WO2016098890A1 - グラファイト積層体、グラファイト積層体の製造方法、熱輸送用構造物およびロッド状の熱輸送体 - Google Patents
グラファイト積層体、グラファイト積層体の製造方法、熱輸送用構造物およびロッド状の熱輸送体 Download PDFInfo
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Definitions
- the present invention relates to a graphite laminate, a method for producing a graphite laminate, a heat transport structure, and a rod-shaped heat transport body.
- Polymer-fired graphite sheets have excellent heat dissipation properties, and have been used as heat dissipation components in semiconductor devices and other heat-generating components mounted on various electronic devices such as computers or electrical devices. It was.
- a graphite sheet as a heat radiating component is often used by being attached to the entire back surface of a liquid crystal display of a computer device, for example.
- heat pipes are used as parts for transporting heat generated by CPUs in large quantities.
- the heat pipe has a structure in which a liquid is enclosed in a copper pipe, and when the liquid is heated and vaporized in the heating section, it takes heat of vaporization from the electronic equipment, thereby cooling the electronic equipment. To do.
- the vaporized gas moves to the cooling unit and liquefies, and then the liquid returns to the heating unit again to cool the electronic device. That is, in the heat pipe, vaporization and liquefaction are repeatedly performed, whereby the electronic device can be efficiently cooled.
- efforts are being made to devise pipe cross-sectional shapes and sizes, pipe materials, and hydraulic fluid materials in order to deal with smaller and higher-power devices such as smartphones. .
- Patent Document 1 a heat dissipation sheet obtained by laminating a graphite film with an adhesive material to form a graphite block and slicing the graphite block is described.
- the technique described in Patent Document 1 is to obtain a flexible heat-dissipating sheet oriented in the thickness direction by once laminating a graphite film oriented in the plane direction into a graphite block and slicing it thinly in the laminating direction. Yes, different from the present invention.
- the heat pipe is a cycle in which the working fluid absorbs heat at the high temperature site and evaporates, and the vaporized gas moves through the cavity to the low temperature site, aggregates and becomes liquid, and returns to the high temperature part.
- the operating principle is to transport heat.
- the heat pipe may not function in an instant if it becomes hot even temporarily. For this reason, the heat pipe has a problem that the heat transport capability suddenly decreases at a specific temperature, so that it cannot be used stably, and a problem that the use temperature is limited.
- the present inventors use a graphite sheet laminate as a heat pipe raw material in producing a heat transporter.
- the advantages of the graphite sheet are that i) it can be made smaller, thinner and lighter, and ii) less susceptible to gravity. Therefore, it is common technical knowledge that the graphite sheet is used as a heat radiating member in the state of one non-laminated graphite sheet, and a person skilled in the art has the concept of using a laminated graphite sheet as a heat transporter. There was no. Furthermore, there was no concept of forming the laminate into a desired shape and using it as a raw material for the heat transporter.
- the expected thermal conductivity thermal conductivity of the graphite sheet ⁇ graphite sheet thickness
- the graphite sheet produced from the polymer film as a raw material has low gas permeability, a gas enters between the graphite sheet and the adhesive layer to form a void, and the heat transport finally obtained by the void The strength of the body is lowered, and the heat conduction properties of the finally obtained heat transporter are lowered.
- gas entering in the lamination process of the graphite sheet and the adhesive layer can be mentioned.
- gas entering in the lamination process of the graphite sheet and the adhesive layer can be mentioned.
- a material having a glass transition point of 50 ° C. or lower such as an acrylic adhesive or a rubber sheet
- gas easily enters between the graphite sheet and the adhesive layer during lamination.
- the present invention has been made in view of the above-described conventional problems, and an object of the first invention is to provide a rod-shaped heat transporter that can be used stably without any limitation in use temperature, and a rod-shaped heat transporter.
- An object of the present invention is to provide an electronic device including a heat transporter.
- the object of the second invention is to provide a graphite laminate having a high thermal conductivity and hardly generating voids therein, a method for producing the graphite laminate, and a heat transport structure including the graphite laminate. There is.
- the objective of 3rd invention is providing the manufacturing method of the graphite laminated body with the ease of heat transmission and favorable peel strength, and the said graphite laminated body.
- the heat transporter of the present invention is a rod-shaped heat transporter in order to solve the above-mentioned problems, and the rod-shaped heat transporter has one end of the heat transporter as a high-temperature part.
- the thermal conductivity measured by contacting and contacting the other end with a low-temperature part kept at 20 ° C. satisfies the relationship of formula (1); ⁇ a / ⁇ b > 0.7 Formula (1)
- ⁇ a represents the thermal conductivity when the temperature of the high temperature part is 100 ° C.
- ⁇ b represents the thermal conductivity when the temperature of the high temperature part is 50 ° C.
- the rod-shaped heat transporter of the present invention preferably contains graphite.
- the rod-shaped heat transporter of the present invention has a layered structure.
- the heat transport body of the present invention is a rod-shaped heat transport body in order to solve the above-mentioned problem, and the rod-shaped heat transport body is formed by alternately laminating graphite sheets and adhesive layers.
- the number of laminated graphite sheets is 3 or more and 500 or less.
- the rod-shaped heat transporter of the present invention preferably has a ratio a / b between the minor axis a and the major axis b of the rod-shaped heat transporter of 1/500 or more.
- the rod-shaped heat transporter of the present invention preferably has a rod length L of 4 cm or more.
- the rod-shaped heat transporter of the present invention holds both ends of the heat transporter so that the heat transporter is level with respect to the ground, the one end is removed.
- the center position of the end portion where the holding is removed changes vertically downward from the position before the holding is released by 10% or less of the length L of the rod.
- the rod-shaped heat transporter of the present invention is preferably used as a heat pipe.
- the rod-shaped heat transporter of the present invention is a rod-shaped heat transporter used by being incorporated inside an electronic device in order to solve the above-mentioned problems, and the heat transporter includes a graphite component.
- one end of the heat transporting body is connected to a heating element, and the other end is connected to a low-temperature portion having a temperature lower than that of the heating element, and is used as a thermal highway.
- An electronic device is an electronic device including a heating element, a low temperature part that is lower in temperature than the heating element, and a thermal highway in order to solve the above-described problem. It is the rod-shaped heat transporter of the invention.
- the graphite laminate of the present invention is a graphite laminate including alternately laminated graphite sheets and adhesive layers, and the adhesive layer comprises a thermoplastic resin and a heat
- the adhesive layer contains at least one of curable resins, and the adhesive layer has a water absorption of 2% or less and a thickness of less than 15 ⁇ m, and is included in the graphite laminate.
- the number of laminated graphite sheets is 3 or more.
- the graphite laminate of the present invention is a graphite laminate including graphite sheets and adhesive layers that are alternately laminated in order to solve the above-described problems, and the adhesive layer includes a thermoplastic resin and heat.
- the adhesive layer includes at least one resin among curable resins, the adhesive layer has a thickness of less than 15 ⁇ m, and the number of the graphite sheets included in the graphite laminate is three or more.
- the graphite laminate has a water absorption of 0.25% or less.
- thermoplastic resin and the thermosetting resin preferably have a glass transition point of 50 ° C. or higher.
- the graphite sheet preferably has a thermal conductivity in the plane direction of 1000 W / (m ⁇ K) or more.
- the graphite laminate of the present invention preferably has a shape bent at at least one bent portion of the graphite laminate.
- the graphite laminate of the present invention has a surface defined by an X axis and a Y axis perpendicular to the X axis, and a graphite sheet and an adhesive layer overlap the surfaces.
- the graphite laminate is a graphite laminate that is alternately laminated in the direction of the Z axis that intersects the surface perpendicularly,
- the graphite laminate has a shape bent at at least two bent portions of the graphite laminate,
- Each of the bent portions is any of the following (a) to (c): (A) a first bent portion obtained by bending the graphite laminate toward the X-axis direction or the Y-axis direction; (B) a second bent portion obtained by bending the graphite laminate toward the Z-axis direction; (C) A third bent portion in which the graphite laminate is bent in the X-axis direction or the Y-axis direction and is bent in the Z-axis direction.
- the graphite laminate of the present invention has a surface defined by an X axis and a Y axis perpendicular to the X axis, and a graphite sheet and an adhesive layer overlap the surfaces.
- it is a graphite laminate that is alternately laminated in the direction of the Z axis that intersects the surface perpendicularly
- the graphite laminate has a shape bent at at least one bent portion of the graphite laminate, Each of the bent portions is characterized by the following (c): (C) A third bent portion in which the graphite laminate is bent in the X-axis direction or the Y-axis direction and is bent in the Z-axis direction.
- the graphite laminate of the present invention after fixing one end of the graphite laminate so that the graphite laminate is horizontal to the ground, the graphite laminate is at a position 4 cm away from the fixed end.
- the displacement of the cross section is preferably 15 mm or less.
- the heat transport structure of the present invention is a heat transport structure comprising the graphite laminate of the present invention and a heating element in order to solve the above-mentioned problems, and the graphite laminate Is characterized in that it is connected to a high temperature part that is heated by the heat generated by the heating element and a low temperature part that is lower than the high temperature part.
- a method for producing a graphite laminate of the present invention is a method for producing a graphite laminate comprising alternately laminated graphite sheets and an adhesive layer in order to solve the above-described problem, Laminating step of alternately laminating the adhesive layers to form a laminate, and pressurizing the laminate, or heating and pressurizing, to adhere the graphite sheet and the adhesive layer, and And a bonding step of forming a graphite laminate.
- the adhesive layer contains at least one of a thermoplastic resin and a thermosetting resin and has a water absorption rate of 2% or less. It is preferable that
- the adhesive layer preferably has an adhesive strength at 25 ° C. of 1 N / 25 mm or less.
- the adhesion step preferably includes a bent portion forming step of forming a graphite laminate having at least one bent portion that bends the graphite laminate.
- the laminating step includes the surface of the graphite sheet and the adhesive layer having a surface defined by an X axis and a Y axis perpendicular to the X axis.
- the bent portion forming step preferably includes at least one of the following bent portion forming steps (d) to (h) for forming a graphite laminate having two or more bent portions: (D) The heated and pressurized laminate is cut in the Z-axis direction, and the graphite laminate is cut out from the laminate, so that the graphite laminate has the X-axis direction or the Y-axis.
- Bending part forming step (G) A precursor of a graphite laminate that is cut in the Z-axis direction and bent from the laminate toward the X-axis direction or the Y-axis direction. After cutting out, by pressing the precursor of the graphite laminate with a bending jig having a bent shape, the graphite laminate is directed toward the X-axis direction or the Y-axis direction.
- a fourth bent portion forming step that forms a third bent portion that is bent and bent toward the Z-axis direction; (H) Pressing the heated and pressurized laminate with a pressure jig having a bent shape to bend the laminate toward the Z-axis, and then By cutting obliquely with respect to the Z-axis direction and cutting out the graphite laminate from the laminate, the graphite laminate is bent toward the X-axis direction or the Y-axis direction, and A fifth bent portion forming step of forming a third bent portion bent in the Z-axis direction.
- the laminating step includes the surface of the graphite sheet and the adhesive layer having a surface defined by an X axis and a Y axis perpendicular to the X axis.
- the bent portion forming step preferably includes at least one of the following bent portion forming steps (g) and (h) for forming a graphite laminate having one or more bent portions: (G) A precursor of a graphite laminate that is cut in the Z-axis direction and bent from the laminate toward the X-axis direction or the Y-axis direction.
- the graphite laminate After cutting out, by pressing the precursor of the graphite laminate with a bending jig having a bent shape, the graphite laminate is directed toward the X-axis direction or the Y-axis direction.
- a fourth bent portion forming step that forms a third bent portion that is bent and bent toward the Z-axis direction; (H) Pressing the heated and pressurized laminate with a pressure jig having a bent shape to bend the laminate toward the Z-axis, and then By cutting obliquely with respect to the Z-axis direction and cutting out the graphite laminate from the laminate, the graphite laminate is bent toward the X-axis direction or the Y-axis direction, and A fifth bent portion forming step of forming a third bent portion bent in the Z-axis direction.
- the graphite laminate of the present invention is a graphite laminate including graphite sheets and adhesive layers that are alternately laminated in order to solve the above-described problems, and the adhesive layer includes a thermoplastic resin and a heat It contains at least one resin among curable resins, and the number of laminated graphite sheets contained in the graphite laminate is 3 or more, and the graphite sheet and the adhesive layer have 50 interfaces. % Or more is characterized by being in close contact with each other.
- the method for producing a graphite laminate of the present invention includes a lamination step of obtaining a laminate by alternately laminating a plurality of adhesive layer materials, which are materials of the adhesive layer, and graphite sheets.
- the adhesive layer material includes at least one of a thermoplastic resin and a thermosetting resin.
- the temperature of the adhesive layer material is [(adhesion At least a first pressurization is performed to pressurize the laminate before reaching the melting temperature of the layer material (-20 ° C.), and in the first pressurization, the adhesive layer material is transformed into the graphant.
- the laminate is pressurized so that it is not thermally fused to the sheet, and in the bonding step, at least after the temperature of the adhesive layer material becomes [(melting temperature of adhesive layer material) ⁇ 20 ° C.] or higher,
- a second pressurization is performed to pressurize the object. In the second pressurization, the laminate is pressed so that the adhesive layer material is thermally fused to the graphite sheet.
- the method for producing a graphite laminate of the present invention includes a lamination step of obtaining a laminate by alternately laminating a plurality of adhesive layer materials, which are materials of an adhesive layer, and graphite sheets.
- the rod-like heat transporter of the present invention (first invention) has an effect that it can be used in a wide range of temperatures.
- the present invention (second invention) has an effect that it is possible to realize a graphite laminate having high thermal conductivity and hardly generating voids therein, and a method for producing the graphite laminate.
- the present invention (the first invention) has an effect that each layer can be laminated satisfactorily and each layer can be cut satisfactorily during the production of the graphite laminate.
- the present invention (the third invention) has an effect that it is possible to realize a graphite laminate having good heat transfer and good peel strength and a method for producing the graphite laminate.
- FIG. 1 It is a figure which shows an example of the preparation process of the graphite composite film by a sticker process.
- (A) And (b) is a figure which shows an example of arrangement
- (A) is a side view of a rod-shaped heat transporter
- (b) is a cross-sectional view of the rod-shaped heat transporter.
- the present invention is a rod-shaped heat transporter, and the rod-shaped heat transporter has one end of the heat transporter brought into contact with a high-temperature part and the other end maintained at 20 ° C. It is a rod-shaped heat transporter satisfying the relationship of the formula (1) in the thermal conductivity measured by contacting with a low temperature part.
- Formula (1) In the formula (1), ⁇ a is the thermal conductivity when the temperature of the hot site is 100 ° C., lambda b represents the thermal conductivity when the temperature of the hot site is 50 ° C..
- the heat pipe can transport heat by directly connecting a high temperature part of the electronic device (a heat generating part such as a CPU or near the heat generating part) and a low temperature part (a part having a lower temperature than the high temperature part) of the electronic device. It is used as a thermal highway.
- the problem with using a heat pipe as a thermal highway is that the heat generated in the cavity of the heat pipe evaporates and disappears when the heat generation amount of the CPU suddenly increases and the temperature of the electronic device rises rapidly.
- the electronic equipment cannot be cooled. This is called dryout and is an unavoidable problem as long as the heat pipe is used for heat transport.
- the present inventors thought that the problem of dry-out could be avoided by providing a thermal highway of a different principle that does not require hydraulic fluid. If a rod-shaped material having no cavity or hydraulic fluid is used as the thermal highway, the problem of dryout can be avoided. Further, the rod-shaped material needs to have an ability to transport heat to the rod-shaped material itself. Therefore, the inventors focused on the graphite material, molded it into a rod shape, and used it as a thermal highway as an alternative to a heat pipe to evaluate the heat transport capability. It was also found that it has excellent heat transport capability.
- Graphite materials are used as negative electrode materials and lubricants for lithium ion batteries. Moreover, the graphite material is used as a heat dissipation sheet for electronic equipment. The graphite material used as the heat dissipation sheet is thin and has low stiffness.
- the present inventors dared to laminate a thin and supple heat-dissipating sheet that is used as a heat-dissipating material as it is (layered structure). Then, the laminate was molded into rods of various shapes, hardnesses and sizes considered to be suitable for use as a thermal highway, and the heat transport capability of the rods was evaluated.
- the present inventors have shown that the rod exhibits extremely excellent heat transport capability, and at the same time, does not cause dryout at all.
- the rod When used as a thermal highway, the rod always has a constant heat transport regardless of the temperature of the heat generating portion. I found out that I can. From this knowledge, it was found that graphite can be suitably used as a material for the thermal highway.
- FIG. 24 is a diagram in which the rod-shaped heat transporter 301 of the present invention is arranged on a plate 303 inside the case 304 of the smartphone and used as a thermal highway.
- the heat generated by the heat generating part such as the first CPU 302 can be prevented from being transmitted to the second CPU 305 having low heat resistance, and the heat can be directly transferred from the heat generating element to the low temperature part.
- the heat transport body of the present invention needs to be rod-shaped.
- the rod shape is a so-called uniaxially elongated rod shape, and the cross-sectional shape of the rod is not particularly limited, and may be, for example, a rectangle, a circle, an ellipse, or a polygon.
- the heat transporter of the present invention is in the form of a rod that can be used as a thermal highway
- the size (long) of a preferred cross section of the rod cross section perpendicular to the major axis direction of the rod
- the ratio of the axis to the minor axis) and the length of the rod will be described below.
- FIG. 29A is a side view of the rod-shaped heat transporter 601
- FIG. 29B is a cross-sectional view of the rod-shaped heat transporter 601 at the broken line in FIG. 29A.
- the rod-shaped heat transporter 601 has a length L toward the long axis direction.
- the length of the short axis is a
- the length of the long axis is b.
- a / b is 1/500 or more, where a is the short axis of the cross section of the rod and b is the long axis. It is more preferable that a / b is 1/200 or more from the viewpoint that the temperature difference between arbitrary points in the cross section of the rod becomes small and the efficiency of heat transport increases, and it is 1/100 or more. Is more preferable.
- a / b is defined by the point where the difference between a and b is the largest.
- the length L of the rod is preferably 4 cm or more.
- the length of the rod depends on the size of the smartphone or tablet used, it is preferable from the viewpoint of heat transport to carry heat away from the heat generating part. It is preferable that the length is sufficiently long so that a low-temperature portion sufficiently away from the surface can be directly connected.
- the ratio L / b between the long axis b and the rod length L is determined when the heat is to be carried to a specific place (for example, a graphite sheet, metal, or heat sink in an electronic device (for example, a notebook computer)). Or when using a rod-shaped heat transport body together with a graphite sheet, a metal plate, etc., it is preferable that it is 5 or more.
- L / b is more preferably 10 or more from the viewpoint that the occupied area in the electronic device by the heat pipe can be narrowed, and more preferably 20 or more.
- the upper limit value of L / b is not particularly limited, but is 100 or less (more specifically, 1 to 100) when heat is diffused on the surface and escaped to the air or the like like like a smartphone or a tablet terminal. It is preferably 10 or less (more specifically 1 to 10), more preferably 5 or less (more specifically 1.2 to 5).
- the length of the major axis b is not particularly limited, but is preferably the same as the length of the short side of the heat source or longer than the length of the short side of the heat source. If it is the said structure, heat can be efficiently conveyed from a heat source.
- the heat transport body of the present invention can be represented by the difficulty of deformation (deformation rate).
- the deformation rate is measured by the following method. As shown in FIG. 26 (1), the rod-shaped heat transporter 301 is parallel (horizontal) to the ground, and both ends of the rod-shaped heat transporter 301 are connected to the first clamp 312 and the second clamp 313. Then, as shown in FIG. 26 (2), the second clamp 313 is removed.
- the deformation rate of the rod-shaped heat transporter 301 is defined.
- the deformation rate of the rod-shaped heat transporter of the present invention is 10% or less, and the rod-shaped heat transporter of the present invention is hard.
- the rod-like heat transporter of the present invention is a hard rod from the viewpoint that the strength of the heat transporter itself can be secured.
- the rod-shaped heat transporter invented by the present inventors does not dry out unlike a conventional heat pipe. Therefore, this can be expressed by the thermal conductivity of the heat transporter. That is, the rod-shaped heat transporter of the present invention has a heat measured by bringing one end of the heat transporter into contact with a high temperature part and the other end in contact with a low temperature part kept at 20 ° C. It is a rod-shaped heat transporter that satisfies the relationship of formula (1) in terms of conductivity.
- ⁇ a represents the thermal conductivity when the temperature of the hot region is 100 ° C.
- lambda b represents the thermal conductivity when the temperature of the hot region is 50 ° C..
- the measurement of thermal conductivity can be performed with a measuring apparatus as shown in FIG. In FIG. 1)
- the end 328 of the rod-shaped heat transporter 301 is brought into contact with running water 323 (low temperature portion), and the temperature of the end 328 is kept at 20 ° C. 2)
- the heater 322 (high temperature part) is attached to the end 327 of the rod-shaped heat transporter 301 (in other words, the end 327 is brought into contact with the heater 322 (high temperature part)).
- a thermocouple 325 is attached where the end 327 and the rod-shaped heat transporter 301 are in contact, and a thermocouple 326 is attached where the running water 323 and the end 328 are in contact.
- the output Q of the heater 322 adjusted so that the high temperature part becomes 100 ° C. and the output Q of the heater 322 adjusted so that the high temperature part becomes 50 ° C. are obtained, respectively, ⁇ a when the high temperature part is 100 ° C., Further, ⁇ b when the high temperature part is 50 ° C. is obtained.
- the reason for using a thermal conductivity lambda a time is 100 ° C. is, if it is a conventional heat pipe, if the high-temperature portion was adjusted heater output so that 100 ° C., hydraulic fluid is heated to near boiling This is because it tends to cause dryout at a high temperature region, and a phenomenon in which the amount of heat transport rapidly decreases is observed.
- the reason for using the thermal conductivity ⁇ b when the temperature of the high temperature part is 50 ° C. is that when the heater output is adjusted so that the high temperature part becomes 50 ° C. for a conventional heat pipe, This is because no dry out occurs.
- the thermal conductivity ratio ⁇ a / ⁇ b measured in this way is ⁇ a / ⁇ b > 0.7.
- the heat transporter of the present invention does not cause dryout.
- the heat transporter of the present invention is capable of constant heat transport regardless of the heater output, but considering a slight decrease in heat transport capacity due to factors other than dryout, ⁇ a / ⁇
- Lambda a heat transfer body of the present invention is preferably at least 320W / mK, more 400W / mK is more preferable.
- Lambda b of the heat transport body is preferably at least 400W / mK, more preferably at least 500 W / mK.
- a method for obtaining a rod-shaped heat transporter satisfying the relationship of the above formula (1) a method using graphite (graphite component) as the material thereof can be mentioned.
- a method of forming into a rod shape using a graphite material for example, a) A method of pressing a graphite sheet after pulverizing and filling a mold, b) A method of pressing after pressing into a box shape while bending the graphite sheet and, if necessary, the adhesive layer into an arbitrary shape, c) A method of alternately stacking graphite sheets and adhesive layers, heating and / or pressurizing, bonding the graphite sheets and adhesive layers, and cutting the laminate into a rod shape, etc.
- the method c) is preferable because the rod-shaped heat transporter can be easily designed in the size and shape of the rod and excellent in thermal conductivity.
- a rod-shaped heat transporter having a layered structure can be obtained.
- the graphite sheet to be used is not particularly limited, and a polymer graphite sheet, a graphite sheet obtained by expanding natural graphite as a raw material, or the like can be used. Since the high-molecular graphite sheet has high strength and high thermal conductivity, higher strength in the rod-shaped heat transporter and higher heat transport capability can be realized. preferable.
- the method for producing a graphite sheet in the present invention is not particularly limited.
- a first method for producing a graphite sheet in the present invention there is a method of expanding natural graphite as a raw material. Specifically, after graphite powder is immersed in an acid (for example, sulfuric acid) to produce a graphite intercalation compound, the graphite intercalation compound is heat-treated and foamed to peel off the graphite layer. After peeling off the graphite layer, the graphite layer is washed to remove the acid to obtain a thin film formed of graphite powder.
- a graphite sheet can be obtained by further rolling the thin film obtained by such a method.
- a method of producing a polymer-based graphite sheet by heat-treating a polymer film for example, polyimide resin
- a polymer film for example, polyimide resin
- the polymerized film as a starting material is preheated to a temperature of about 1000 ° C. under reduced pressure or in an inert gas atmosphere to be carbonized, thereby forming a carbonized film.
- the carbonized film is heat-treated at a temperature of 2800 ° C. or higher in an inert gas atmosphere to be graphitized to obtain a graphite sheet having a good graphite crystal structure and excellent thermal conductivity. be able to.
- the thermal conductivity in the plane direction of the graphite sheet in the present invention is preferably 1000 W / (m ⁇ K) or more, more preferably 1100 W / (m ⁇ K) or more, and 1200 W / (m ⁇ K). More preferably, it is more preferably 1300 W / (m ⁇ K) or more.
- thermosetting resin or a thermoplastic resin can be used for the adhesive layer.
- thermosetting resin the same thermosetting resin as described in the column of (Type of adhesive layer) in [Embodiment B] can be used.
- thermoplastic resin the same thermoplastic resin as described in the column of (Type of adhesive layer) in [Embodiment B] can be used.
- the thermoplastic resin and the thermosetting resin preferably have a glass transition point of 50 ° C. or higher, more preferably 60 ° C. or higher, and more preferably 70 ° C. or higher. More preferably, the temperature is higher than or equal to ° C. If the glass transition point is 50 ° C. or higher, air can be better prevented from entering the graphite laminate. In addition, it is preferable to use a material having a glass transition point of 50 ° C. or higher, such as an acrylic adhesive or a rubber sheet, because the strength of the adhesive layer is strong and the characteristics of the adhesive layer tend not to vary. Examples of the material having such a glass transition temperature include PET (polyethylene terephthalate), PS (polystyrene), and PC (polycarbonate).
- the surfaces are alternately stacked.
- stacking an adhesive sheet in a multilayer can be mentioned.
- a graphite adhesive sheet is prepared.
- the graphite adhesive sheet can be produced by applying an adhesive resin or laminating an adhesive film.
- the adhesive layer material (varnish) has no tack after application from the viewpoint of preventing air from entering the graphite laminate. It is preferable.
- the adhesive layer is difficult to be charged if the dielectric constant of the adhesive layer is low, so the adhesive layer is stably fixed to the transport machine by electrostatic force. it can.
- the dielectric constant of the adhesive layer is not particularly limited, but is preferably 1.0 to 5.0, more preferably 2.0 to 4.0, and more preferably 2.5 to 3.6. If the dielectric constant of the adhesive layer is 1.0 to 5.0, the adhesive layer is repelled by static electricity and easily separated, which is preferable as a thermal highway.
- the electrical conductivity of the graphite sheet in the present invention is not particularly limited, but is preferably 1000 to 25000 S / cm, more preferably 2000 to 20000 S / cm, more preferably 5000 to 18000 S / cm, and more preferably 10,000 to 17000 S / cm. .
- the electrical conductivity of the graphite sheet is 1000 to 25000 S / cm, it is possible to ensure appropriate adhesion and moderate slipperiness between the graphite sheet and the adhesive layer, and to superimpose the adhesive layer and the graphite sheet ( In particular, it is excellent as a thermal highway because of excellent superposition with a thin adhesive layer.
- the graphite sheet and the adhesive layer are adhered by heating and pressurizing (in other words, compression) to form a graphite laminate.
- heating and pressurizing include laminating and pressing.
- adhesion by pressing is preferable. If it is a press, even a multi-layered laminate of 10 layers or more can be bonded together.
- pressurization is performed for several seconds or more while heating, the softening of the adhesive layer and the effect of pressurization can suppress air from being caught in the graphite laminate. The contact thermal resistance between them can be reduced.
- the heating temperature and pressurizing pressure are not particularly limited, and can be appropriately selected depending on the material constituting the adhesive layer.
- the compression ratio of the laminate by heating and pressing is not particularly limited, but is preferably less than 1, more preferably 0.97 or less, more preferably 0.96 or less, and 0.95. Or less, more preferably 0.92 or less, and even more preferably 0.90 or less. If the compression ratio (thickness of the graphite laminate / thickness of the laminate as a raw material) is smaller than 1, the adhesive layer is deformed at the time of lamination, so that the graphite sheets easily come into contact with each other, and theoretical heat conduction is achieved. A close graphite stack can be obtained.
- the number of graphite sheets included in the graphite laminate is 3 or more and 500 or less, and preferably 5 or more and 400 or less.
- the graphite laminate used in the present invention is such that, as described in Patent Document 1, 1000 or more layers of graphite sheets are laminated, and this is sliced in the vertical direction to obtain sheet-like graphite again.
- the purpose of producing such a laminate once in the present invention is to obtain a rod-shaped heat transport body having a shape, strength and size necessary for transporting heat in a desired direction within the surface. . Therefore, the graphite laminate used in the present invention is different from the technique described in Patent Document 1 intended for the vertical orientation.
- the graphite laminated body used in the present invention does not require an excessive number of laminated graphite sheets as in the technique described in Patent Document 1 in which the final product is a sheet.
- the heat transporter is cut into a desired shape and size suitable for use as a thermal highway from this laminate in the form of a rod.
- This method can easily form a rod having a bent portion to be described later. That is, it can be manufactured by punching the obtained laminate into a rod shape having a bent portion.
- the cutting can be performed using a blade saw such as a cutter or an outer peripheral blade, a laser, a water jet, a wire saw, or the like.
- a graphite laminate obtained by heating and pressurizing an object to be laminated is placed between members using a pressing jig in which a convex member and a concave member form a pair, and then added.
- a graphite laminate having a bent portion can be obtained and then manufactured by cutting into a rod shape.
- the rod-shaped heat transporter of the present invention may have a bent shape having at least one bent portion.
- the heat generated from the heating element inside the electronic device can be made into a rod shape that can be efficiently transported directly to the low-temperature part that is the destination of heat transport, and the freedom of rod shape design
- the degree increases. This is particularly effective when the low temperature part and the heat source cannot always be connected linearly due to the specifications of the electronic device. That is, the degree of freedom in the arrangement relationship between the heat source and the lower temperature portion can be increased.
- the heat transport body can be freely designed into a rod shape suitable for the thermal highway.
- the number of bent portions formed on the rod-shaped heat transporter is not particularly limited, and a desired number can be formed.
- the angle at which the bent part bends is not particularly limited.
- the bent portion may be bent with a curvature radius of 2 mm or more, a curvature radius of 5 mm or more, a curvature radius of 8 mm or more, a curvature radius of 10 mm or more, or a curvature radius of 20 mm or more.
- the maximum value of the radius of curvature is not particularly limited, and may be, for example, 100 mm, 90 mm, 80 mm, 70 mm, 60 mm, 50 mm, 40 mm, 30 mm, or 20 mm. Of course, the maximum value of the radius of curvature may be a value larger than 100 mm.
- the rod-shaped heat transporter is coated with a resin (for example, PET (polyethylene terephthalate), PE (polyethylene) or PI (polyimide)), or a metal (for example, copper, nickel, or gold). It is preferable. Since the graphite sheet is a layered compound, powder falling off easily occurs due to rubbing or the like. And since a graphite sheet has electrical conductivity, when powder fall occurs, a short circuit of an electronic device will be generated.
- a resin for example, PET (polyethylene terephthalate), PE (polyethylene) or PI (polyimide)
- a metal for example, copper, nickel, or gold
- the rod-shaped heat transporter by covering the rod-shaped heat transporter, powder fall off from the graphite sheet can be suppressed, thereby preventing occurrence of a short circuit of the electric device. Moreover, by covering the rod-shaped heat transporter, the strength of the rod-shaped heat transporter is improved, and the occurrence of delamination can be suppressed.
- a metal is preferable from the viewpoint of improving thermal conductivity and strength.
- the method for coating the rod-shaped heat transporter with a metal is not particularly limited, and examples thereof include vapor deposition, sputtering, or plating. From the viewpoint of forming a metal layer having higher adhesion, plating is performed. Treatment is preferred.
- the thickness of the coating film covering the rod-shaped heat transporter is not particularly limited, but is preferably 0.5 ⁇ m or more and 15 ⁇ m or less, more preferably 1 ⁇ m or more and 10 ⁇ m or less, and 2 ⁇ m or more and 7 ⁇ m or less. More preferably.
- the thickness of the coating film is 0.5 ⁇ m or more, the protection property of the rod-shaped heat transporter is improved, and the rod-shaped heat transporter becomes strong against mechanical scratching or rubbing.
- the thickness of a coating film is 15 micrometers or less, the heat conductivity of a rod-shaped heat transport body can be made high.
- the heat transporter of the present invention can be used as a conventional heat pipe substitute and can be used as a thermal highway in an electronic device.
- One end of the rod-shaped heat transporter is connected to a heating element such as a CPU, and the other end is connected to the cooling unit.
- a heating element such as a CPU
- the other end is connected to the cooling unit.
- part is a site
- the heat transporter of the present invention can be suitably used to transport heat from one point to another point in the same plane.
- the rod-shaped heat transporter of the present embodiment has the effect of being excellent in heat transport stability and not being limited by the temperature environment in which it is used because the amount of heat that can be transported is constant regardless of the temperature change of the heating element.
- the rod-shaped heat transporter of the present embodiment is preferably used as a heat transporter used in smartphones, tablets, fanless notebook computers, etc., which generate a larger amount of heat from the CPU due to downsizing and higher performance. Can do.
- the rod-shaped heat transporter of the present embodiment is used as a substitute for a conventional heat pipe, it not only has excellent heat transport capability, but also does not cause dryout due to changes in use conditions.
- the graphite laminate according to the present embodiment is a graphite laminate including graphite sheets and adhesive layers that are alternately laminated (or a graphite laminate in which graphite sheets and adhesive layers are alternately laminated).
- the adhesive layer may include at least one of a thermoplastic resin and a thermosetting resin. Furthermore, the adhesive layer may have a water absorption of 2% or less and a thickness of less than 15 ⁇ m.
- the number of the graphite sheets included in the graphite laminate may be three or more.
- the graphite laminate may be obtained by further compressing a laminate in which the graphite sheet and the adhesive layer are alternately laminated.
- the thickness of the above-mentioned adhesive layer is intended to be the thickness of the adhesive layer in a state of being incorporated in the finished graphite laminate, and before being incorporated in the finished graphite laminate.
- the thickness of the adhesive layer is not intended.
- the thickness of the adhesive layer in a state of being incorporated into the finished graphite laminate is substantially the same as the thickness of the adhesive layer before being incorporated into the finished graphite laminate.
- the graphite laminate of the present embodiment is a graphite laminate including alternately laminated graphite sheets and adhesive layers (or a graphite laminate in which graphite sheets and adhesive layers are alternately laminated).
- the adhesive layer may include at least one of a thermoplastic resin and a thermosetting resin. Furthermore, the adhesive layer may have a water absorption of 2% or less.
- the graphite laminate may be obtained by compressing a laminate in which the graphite sheet and the adhesive layer are alternately laminated. The number of the graphite sheets included in the graphite laminate may be three or more. In the graphite laminate, the adhesive layer may have a thickness of less than 15 ⁇ m.
- the graphite laminate of the present embodiment is a graphite laminate including alternately laminated graphite sheets and adhesive layers (or a graphite laminate in which graphite sheets and adhesive layers are alternately laminated).
- the adhesive layer may include at least one of a thermoplastic resin and a thermosetting resin. Furthermore, the adhesive layer may have a thickness of less than 15 ⁇ m.
- the number of the graphite sheets included in the graphite laminate may be three or more.
- the graphite laminate may have a water absorption rate of 0.25% or less (preferably 0.2% or less, more preferably 0.1% or less).
- “obtained by compression” means that the total thickness of the material after compression is thinner than the total thickness of the material before compression. At this time, those in which the components of the adhesive layer are infiltrated into the surface of the graphite sheet are also included in “obtained by compression”. Whether or not the graphite laminate is obtained by compression is determined by i) comparing the thickness of the graphite laminate before and after the compression treatment, or ii) the graphite laminate by SEM (scanning electron microscope). This can be confirmed by observing the interface between the layers. For example, in the case of the above method ii), the interface between the graphite sheet and the adhesive layer in the graphite laminate is observed by SEM. If the interface is not straight, the graphite laminate is obtained by compression. It can be determined that it is a thing.
- the graphite laminate of the present invention may have a shape bent at at least one bent portion. That is, the graphite laminate of the present invention may be a product of bending the graphite laminate of the present invention before bending at a bent portion.
- FIG. 1 is a diagram showing a basic structure of a graphite laminate.
- each of the graphite sheet 5 and the adhesive layer 6 constituting the graphite laminate 1 has a surface defined by an X axis and a Y axis perpendicular to the X axis.
- the graphite sheet 5 and the adhesive layer 6 are laminated
- the angle at which the X axis and the Y axis intersect is 90 °.
- the state where the surfaces overlap means that at least a part of the surface of the graphite sheet 5 and at least the surface of the adhesive layer 6 when the laminate 1 is viewed in the Z-axis direction as shown in FIG. A part is intended to overlap.
- the shape of the surface of the graphite sheet 5 and the shape of the surface of the adhesive layer 6 may be the same or different, but from the viewpoint of realizing a desired effect better, graphite
- the shape of the surface of the sheet 5 and the shape of the surface of the adhesive layer 6 are preferably the same.
- the shape of the surface of the graphite sheet 5 and the shape of the surface of the adhesive layer 6 may be square.
- the direction in which one side defining the surface extends can be defined as the X-axis direction
- the direction in which another side that intersects the side extends can be defined as the Y-axis direction.
- the shape of the surface of the graphite sheet 5 and the shape of the surface of the adhesive layer 6 may be rectangular.
- the direction in which the short side of the rectangle extends can be the X-axis direction
- the direction in which the long side of the rectangle extends can be the Y-axis direction.
- the shape of the surface of the graphite sheet 5 and the shape of the surface of the adhesive layer 6 may be other than a square or a rectangle.
- the longest direction of the surface can be the Y-axis direction, and the direction orthogonal to the Y-axis can be the X-axis direction.
- the number of graphite sheets contained in the graphite laminate may be 3 or more, more preferably 5 or more, more preferably 10 or more, and more preferably 15 or more. More preferably, there are 20 or more layers.
- the upper limit of the number of stacked layers is not particularly limited, but may be 1000 layers or less, 500 layers or less, 200 layers or less, 100 layers or less, 80 layers or less, or 50 layers or less.
- the number of laminated layers is three or more because a graphite laminated body having high heat transport capability and excellent mechanical strength can be obtained.
- the number of adhesion layers included in the graphite laminate is not particularly limited, and can be appropriately set according to the number of graphite sheets.
- two or more adhesive layers as well as one adhesive layer may be disposed between adjacent graphite sheets.
- It may be disposed only on the top surface of the body, only on the bottom surface of the graphite laminate, or may be disposed on both the top surface and the bottom surface of the graphite laminate. It may be disposed only on the uppermost surface, disposed only on the lowermost surface of the graphite laminate, or may be disposed on both the uppermost surface and the lowermost surface of the graphite laminate.
- graphite sheets and adhesive layers are alternately laminated includes (a) a case where one adhesive layer is disposed between adjacent graphite sheets, and (b) adjacent graphite sheets. Both are included when two or more adhesive layers are disposed between them. That is, in the present invention, the adhesive layer may be a laminate of a plurality of adhesive layers.
- the thickness of the graphite laminate (in other words, the length in the direction of the Z axis in FIG. 1) is not particularly limited, but is preferably 0.5 mm or more, more preferably 0.6 mm or more, More preferably, it is 0.7 mm or more, and more preferably 0.8 mm or more. If the thickness of the graphite laminate is 0.5 mm or more, the amount of heat that can be transported increases, and the present invention can also be applied to electronic devices that generate a large amount of heat.
- the upper limit value of the thickness of the graphite laminate is not particularly limited, but may be 10 mm or less, 7.5 mm or less, or 5 mm or less from the viewpoint of thinning the electronic device. It may be 2.5 mm or less, or 1 mm or less.
- a value (Tg / Ta) obtained by dividing the total thickness (Tg) of each graphite sheet by the total thickness (Ta) of each adhesive layer is 4.1 or more and 40 or less (more preferably, 8 0.0 to 40 or less, 4.1 to 27 or less, or 8.0 to 27, and the thickness of the graphite laminate is preferably 0.5 mm or more.
- the graphite sheet has high thermal conductivity, the thickness is as thin as about 80 ⁇ m or less, and the amount of heat that can be transported at one time is not large. Therefore, in order to transport a large amount of heat at a time, it is preferable to laminate the graphite sheets to improve the heat transport capability.
- laminating via an adhesive layer is effective in order to absorb irregularities on the surface of the graphite sheet and reduce the contact thermal resistance between the graphite sheets.
- Tg / Ta is preferably 4.1 or more, and more preferably 8.0 or more.
- Tg / Ta is 4.1 or more, the existence ratio in the graphite laminate of the adhesive layer having a lower thermal conductivity than that of the graphite sheet is suppressed, and high thermal conductivity of the graphite laminate can be realized.
- Tg / Ta is preferably 40 or less, and more preferably 27 or less. If Tg / Ta is 40 or less, irregularities on the surface of the graphite sheet can be absorbed by the adhesive layer, so that the contact thermal resistance between the graphite sheets can be reduced, and the thermal conductivity of the graphite laminate is high. Can be realized. Furthermore, if Tg / Ta is 40 or less, the adhesive force between the graphite sheets becomes good, so that a graphite laminate that can withstand processing such as cutting and bending can be obtained.
- Tg / Ta is preferably in the range of 1 to 50.
- the graphite laminate may have a shape bent at at least one (for example, one or more, or two or more) bent portions provided in the graphite laminate.
- the graphite laminate of the present embodiment can be obtained by bending the graphite laminate before bending at the bent portion.
- heat can be transported by moving the heat generated by the heat source to a lower temperature part.
- the low temperature part and the heat source cannot always be connected linearly. Therefore, by forming a bent portion in the graphite laminate, the heat generated by the heat source can be easily moved to a lower temperature portion, thereby further improving the heat transport capability. . That is, the degree of freedom in the arrangement relationship between the heat source and the lower temperature portion can be increased.
- the number of bent portions formed in the graphite laminate is not particularly limited, and a desired number can be formed.
- the bent portion has no seam.
- heat transfer is improved, and the heat transport capability of the graphite laminate can be improved.
- the term “seam” refers to a seam that divides the structural continuity of one graphite sheet.
- the division that may occur between the graphite sheet and another graphite sheet adjacent to the graphite sheet with the adhesive layer interposed therebetween does not correspond to the “seam” in the present specification.
- the specific shape of the bent portion is not particularly limited, and can be any of the following (a) to (c), for example: (A) a first bent portion obtained by bending the graphite laminate toward the X-axis direction or the Y-axis direction; (B) a second bent portion obtained by bending the graphite laminate toward the Z-axis direction; (C) A third bent portion in which the graphite laminate is bent in the X-axis direction or the Y-axis direction and is bent in the Z-axis direction.
- each of the bent portions is the first bent portion, the second bent portion, or the first bent portion described above. Any one of the three bent portions, or (ii) one or more bent portions may be formed, and each of the bent portions may be the third bent portion described above.
- the structure of the graphite laminated body of this Embodiment is not limited to (i) and (ii).
- the first bent portion and the second bent portion are for bending the graphite laminate before the bending in a plane (in other words, two-dimensionally) at a desired angle
- the third bent portion is The graphite laminate before bending is bent three-dimensionally (in other words, three-dimensionally) at a desired angle.
- FIG. 2 shows an example of a graphite laminate having a first bent portion.
- the graphite laminate 1 is bent toward the X axis and / or Y axis at the bent portion 10 (first bent portion).
- the angle at which the graphite laminate 1 is bent is not limited, and can be bent to a desired angle.
- FIG. 3 shows an example of a graphite laminate having a second bent portion.
- the graphite laminate 1 is bent in the direction of the Z axis at the bent portion 11 (second bent portion).
- the angle at which the graphite laminate 1 is bent is not limited, and can be bent to a desired angle.
- FIG. 4 shows an example of a graphite laminate having a third bent portion.
- the graphite laminate 1 is bent in the direction of the X axis and / or the Y axis at the bent portion 12 (third bent portion) and the direction of the Z axis. It is bent toward.
- the angle at which the graphite laminate 1 is bent is not limited, and can be bent to a desired angle.
- FIG. 5 shows an example of a graphite laminate having a plurality of bent portions.
- the graphite laminate 1 is bent in the direction of the Z axis at the bent portion 11 (second bent portion), and further, the bent portion 10 (first bent portion). ),
- the graphite laminate 1 is bent in the direction of the X-axis. More specifically, the graphite laminate shown in FIG. 5 includes a region 15 extending in the Y-axis direction, a region 16 extending in the Z-axis direction, and a region 17 extending in the X-axis direction. Yes.
- a second bent portion is provided at the boundary between the region 15 and the region 16, and a first bent portion is provided at the boundary between the region 16 and the region 17.
- the angle at which the graphite laminate 1 is bent is not limited, and can be bent to a desired angle.
- the X axis, the Y axis, and the Z axis are defined based on a planar graphite laminate before bending. Even after the graphite laminate is bent, the X axis, the Y axis, and the Z axis defined first can be considered in the same manner as before the bending. That is, the direction in which the graphite sheets are stacked may be considered as the Z axis.
- the axis described as “Y axis” in FIG. 5 corresponds to the Z axis, which is the direction in which the graphite sheets are laminated, and also in the region 17, it is described as “Y axis” in FIG. 5.
- the corresponding axis corresponds to the Z axis, which is the direction in which the graphite sheets are laminated.
- “bend toward the direction of the X-axis” means that the planar graphite laminate before bending spreading in the XY plane is at a desired angle in the XY plane.
- “bend in the direction of the Y-axis” means that a flat graphite laminate before bending extending in the XY plane is desired in the XY plane.
- Is intended to bend in the direction of the Y-axis, and “bend in the direction of the Z-axis” means that the planar graphite laminate before bending that extends in the XY plane has a desired angle.
- a planar graphite laminate before bending that extends in the XY plane is formed at a desired angle in the XY plane.
- the direction of the Z-axis that is bent in the direction of the axis or in the direction of the Y-axis and further bent in the XY plane is perpendicular to the XY plane at a desired angle. It is intended to bend to.
- an unbonded portion in which adjacent graphite sheets are not bonded by an adhesive layer may be formed. Details of the unbonded portion will be described later.
- the angle at which the bent part bends is not particularly limited.
- the bent portion may be bent with a curvature radius of 2 mm or more, a curvature radius of 5 mm or more, a curvature radius of 8 mm or more, a curvature radius of 10 mm or more, or a curvature radius of 20 mm or more.
- the maximum value of the radius of curvature is not particularly limited, and may be, for example, 100 mm, 90 mm, 80 mm, 70 mm, 60 mm, 50 mm, 40 mm, 30 mm, or 20 mm. Of course, the maximum value of the radius of curvature may be a value larger than 100 mm.
- the graphite laminate is preferably coated with a resin (for example, PET (polyethylene terephthalate), PE (polyethylene) or PI (polyimide)), or a metal (for example, copper, nickel, or gold).
- a resin for example, PET (polyethylene terephthalate), PE (polyethylene) or PI (polyimide)
- a metal for example, copper, nickel, or gold.
- the graphite laminate it is possible to suppress powder falling from the graphite sheet, thereby preventing the occurrence of a short circuit of the electric device. Further, by covering the graphite laminate, the strength of the graphite laminate can be improved and the occurrence of delamination can be suppressed.
- a metal is preferable from the viewpoint of improving thermal conductivity and strength.
- the method for coating the graphite laminate with a metal is not particularly limited, and examples thereof include vapor deposition, sputtering, or plating treatment. From the viewpoint of forming a metal layer having higher adhesion, plating treatment is preferable. .
- the thickness of the coating film covering the graphite laminate is not particularly limited, but is preferably 0.5 ⁇ m or more and 15 ⁇ m or less, more preferably 1 ⁇ m or more and 10 ⁇ m or less, and 2 ⁇ m or more and 7 ⁇ m or less. More preferred. If the thickness of the coating film is 0.5 ⁇ m or more, the protective property of the graphite laminate is improved, and the graphite laminate is strong against mechanical scratching and rubbing. Moreover, if the thickness of a coating film is 15 micrometers or less, the heat conductivity of a graphite laminated body can be made high.
- the water absorption rate of the graphite laminate is not particularly limited, but is preferably 0.25% or less, more preferably 0.20% or less, and most preferably 0.10% or less. If the graphite laminate has a water absorption rate of 0.25% or less, the gas generated when the graphite laminate is vaporized when the graphite laminate is manufactured or when the graphite laminate is used as a heat transport mechanism. Since there is little quantity of (outgas), it can prevent that a space
- the graphite laminate is fixed to one end of the graphite laminate so that the graphite laminate is horizontal to the ground, and then to the cross section of the graphite laminate at a position 4 cm away from the fixed end.
- the displacement of the cross section is 15 mm or less, preferably 14 mm or less, more preferably 13 mm or less, more preferably 12 mm or less, more preferably 11 mm or less, and more Preferably it is 10 mm or less, more preferably 9 mm or less, more preferably 8 mm or less, more preferably 7 mm or less, more preferably 6 mm or less, more preferably 5 mm or less, more preferably 4 mm or less, more preferably 3 mm or less, more preferably 2 mm or less, most preferably 1 mm or less.
- the harder the graphite laminate in other words, the smaller the change in the shape of the graphite laminate, the easier the handling of the graphite laminate and the more preferable.
- the graphite sheet in the present invention is not particularly limited, and a polymer graphite sheet, a graphite sheet obtained by expanding natural graphite as a raw material, or the like can be used.
- the polymer-based graphite sheet is preferable because it has high strength and high thermal conductivity, and thus can achieve higher strength and higher heat transport capability in the graphite laminate.
- the manufacturing method of the graphite sheet in this invention is not specifically limited.
- a method for producing a graphite sheet in the present invention there is a method of expanding natural graphite as a raw material. Specifically, after graphite powder is immersed in an acid (for example, sulfuric acid) to produce a graphite intercalation compound, the graphite intercalation compound is heat-treated and foamed to peel off the graphite layer. After peeling off the graphite layer, the graphite layer is washed to remove the acid to obtain a thin film formed of graphite powder. A graphite sheet can be obtained by further rolling the thin film obtained by such a method.
- an acid for example, sulfuric acid
- a method of producing a polymer-based graphite sheet by heat-treating a polymer film for example, polyimide resin
- a polymer film for example, polyimide resin
- the polymerized film as a starting material is preheated to a temperature of about 1000 ° C. under reduced pressure or in an inert gas atmosphere to be carbonized, thereby forming a carbonized film.
- the carbonized film is heat-treated at a temperature of 2800 ° C. or higher in an inert gas atmosphere to be graphitized to obtain a graphite sheet having a good graphite crystal structure and excellent thermal conductivity. be able to.
- the thermal conductivity in the surface direction of the graphite sheet in the present invention is preferably 1000 W / (m ⁇ K) or more, more preferably 1100 W / (m ⁇ K) or more, and 1200 W / (m ⁇ K). More preferably, it is more preferably 1300 W / (m ⁇ K) or more.
- a graphite sheet having a thermal conductivity in the plane direction of 1000 W / (m ⁇ K) or more a graphite laminate having a higher heat transport capability can be obtained.
- a graphite sheet having a thermal conductivity in the plane direction of 1000 W / (m ⁇ K) or more has a thermal conductivity three times or more that of a metal material (eg, copper, aluminum, etc.). Therefore, if the number of graphite sheets contained in the graphite laminate is set so that the heat transport capacity is the same as the configuration using copper or aluminum, the weight of the graphite laminate can be greatly reduced. As a result, it is possible to contribute to weight reduction of the electronic device.
- the thickness of the graphite sheet in the present invention is not particularly limited, but is preferably 10 ⁇ m or more and 200 ⁇ m or less, more preferably 12 ⁇ m or more and 150 ⁇ m or less, more preferably 15 ⁇ m or more and 100 ⁇ m or less, and more preferably 20 ⁇ m or more and 80 ⁇ m or less. It is as follows. If the thickness of the graphite sheet is 10 ⁇ m or more, the number of graphite sheets included in the graphite laminate can be reduced, and the number of adhesive layers having low thermal conductivity can be reduced. Moreover, if the thickness of a graphite sheet is 200 micrometers or less, the high thermal conductivity of a graphite laminated body is realizable.
- the electrical conductivity of the graphite sheet in the present invention is not particularly limited, but is preferably 1000 to 25000 S / cm, more preferably 2000 to 20000 S / cm, more preferably 5000 to 18000 S / cm, and more preferably 10,000 to 17000 S / cm. . If the electrical conductivity of the graphite sheet is 1000 to 25000 S / cm, it is possible to ensure appropriate adhesion and moderate slipperiness between the graphite sheet and the adhesive layer, and to superimpose the adhesive layer and the graphite sheet ( In particular, it is preferable because it is excellent in superposition with a thin adhesive layer.
- the density of the graphite sheet in the present invention is not particularly limited, but is preferably 0.8 g / cm 3 or more, preferably 1.0 g / cm 3 or more, more preferably 1.5 g / cm 3 or more, and 2.0 g / cm. 3 or more is more preferable, and 2.5 g / cm 3 or more is more preferable. If the density of the graphite sheet is 0.8 g / cm 3 or more, it is preferable because the graphite sheet itself is excellent in self-supporting properties.
- the surface roughness of the graphite sheet in the present invention is not particularly limited, but is preferably 5 ⁇ m or less, more preferably less than 2.0 ⁇ m, more preferably 1.5 ⁇ m or less, and more preferably less than 1.0 ⁇ m. If the surface roughness of the graphite sheet is 5 ⁇ m or less, it is possible to ensure appropriate adhesion and moderate slipperiness between the graphite sheet and the adhesive layer, and to superimpose the adhesive layer and the graphite sheet (especially thin). This is preferable because it is excellent in overlaying with an adhesive layer.
- the holes are formed in 0.5% or more of the surface area of the graphite sheet, and it is more preferable that the holes are formed in 1% or more.
- the shape of the hole is not particularly limited, and can be appropriately selected from a perfect circle, an ellipse, a triangle, a quadrangle, and the like.
- Adhesive layer (Type of adhesive layer)
- the adhesive layer in the present invention can use a thermosetting resin or a thermoplastic resin.
- a film-like thing can also be used and a varnish-like thing can also be used.
- thermosetting resin PU (polyurethane), phenol resin, urea resin, melamine resin, guanamine resin, vinyl ester resin, unsaturated polyester, oligoester acrylate, diallyl phthalate, DKF resin (a kind of resorcinol resin),
- examples include xylene resin, epoxy resin, furan resin, PI (polyimide-based) resin, PEI (polyetherimide) resin, PAI (polyamideimide) resin, PPE (polyphenylene ether), and the like.
- an epoxy resin, a urethane resin, and PPE are preferable because of a wide range of material selection and excellent adhesion to the graphite sheet.
- thermoplastic resins acrylic, ionomer, isobutylene maleic anhydride copolymer, AAS (acrylonitrile-acrylic-styrene copolymer), AES (acrylonitrile-ethylene-styrene copolymer), AS (acrylonitrile-styrene copolymer), ABS (acrylonitrile-butadiene-styrene copolymer), ACS (acrylonitrile-chlorinated polyethylene-styrene copolymer), MBS (methyl methacrylate-butadiene-styrene copolymer), ethylene-vinyl chloride copolymer, EVA (ethylene) -Vinyl acetate copolymer), EVA (ethylene-vinyl acetate copolymer system), EVOH (ethylene vinyl alcohol copolymer), polyvinyl acetate, chlorinated vinyl chloride, chlorinated polyethylene, chlorinated polypropylene, Ruboxyvinyl polymer
- the adhesive layer it is preferable to use an aromatic material (for example, a polyester adhesive, polyethylene terephthalate, or the like).
- an aromatic material for example, a polyester adhesive, polyethylene terephthalate, or the like.
- the thermoplastic resin and the thermosetting resin preferably have a glass transition point of 50 ° C. or higher, more preferably 60 ° C. or higher, and more preferably 70 ° C. or higher. More preferably, the temperature is higher than or equal to ° C. If the glass transition point is 50 ° C. or higher, air can be better prevented from entering the graphite laminate. In addition, it is preferable to use a material having a glass transition point of 50 ° C. or higher, such as an acrylic adhesive or a rubber sheet, because the strength of the adhesive layer is strong and the characteristics of the adhesive layer tend not to vary. Examples of the material having such a glass transition temperature include PET (polyethylene terephthalate), PS (polystyrene), and PC (polycarbonate).
- the elastic modulus of the adhesive layer is not particularly limited, but is preferably high (for example, the elastic modulus is 100 MPa or more) from the viewpoint of suppressing variation in thickness at the time of cutting.
- the thickness of the adhesive layer in the present invention may be less than 15 ⁇ m.
- the thickness of the adhesive layer in the present invention is preferably 0.1 ⁇ m or more and less than 15 ⁇ m, and more preferably 1 ⁇ m or more and less than 15 ⁇ m. More specifically, the thickness of the adhesive layer in the present invention is preferably from 0.1 to 10 ⁇ m, more preferably from 1 to 10 ⁇ m, more preferably from 1 to 9 ⁇ m, and more preferably from 1 to 7 ⁇ m. If the thickness of the adhesive layer is less than 15 ⁇ m (more preferably less than 10 ⁇ m), the thermal conductivity of the adhesive layer is much smaller than the thermal conductivity of the graphite sheet.
- the thickness of the adhesive layer is less than 15 ⁇ m (more preferably less than 10 ⁇ m), it is possible to transfer heat well without inhibiting heat transfer between the graphite sheets. If the thickness of the adhesive layer is 1 ⁇ m or more, the adhesive layer can absorb irregularities on the surface of the graphite sheet, reduce the contact thermal resistance between the graphite sheet and the adhesive layer, and efficiently transfer heat. be able to. Moreover, if an adhesive layer is 1 micrometer or more, an adhesive layer can show favorable adhesiveness. Moreover, if it is the thickness of the contact bonding layer mentioned above, the thermal conductivity of a graphite laminated body can be made into the value close
- the water absorption rate of the adhesive layer in the present invention may be 2% or less. More specifically, the water absorption of the adhesive layer in the present invention is more preferably 1.5% or less, more preferably 1.0% or less, more preferably 0.4% or less, and more preferably 0.1% or less. . If the water absorption rate of the adhesive layer is 2% or less, the water contained in the adhesive layer is vaporized and gas (outgas) is generated when the graphite laminate is manufactured or when the graphite laminate is used as a heat transport mechanism. Since the generated amount is small, it is possible to prevent voids from being generated inside the graphite laminate.
- the dielectric constant of the adhesive layer in the present invention is not particularly limited, but is preferably 1.0 to 5.0, more preferably 2.0 to 4.0, and more preferably 2.5 to 3.6. If the dielectric constant of the adhesive layer is 1.0 to 5.0, it is preferable because the adhesive layer is repelled by static electricity and easily separated.
- the adhesive layer preferably exhibits adhesiveness by heating and has adhesiveness in the bonding step. Therefore, as the adhesive layer, a pressure-sensitive adhesive, an adhesive, a polymer film, or the like can be used, but the adhesive strength at 25 ° C. is preferably 1 N / 25 mm or less, and the adhesive strength at 25 ° C. is 0. More preferably, the adhesive layer has an adhesive strength at 25 ° C. of 1 N / 25 mm or less, or an adhesive strength at 25 ° C. of 0.5 N / 25 mm or less. It is preferable that it exhibits adhesiveness by heating.
- the breaking strength of the adhesive layer in the present invention is not particularly limited, but is preferably 0.1 to 10 GPa, more preferably 0.2 to 5.0 GPa, more preferably 0.2 to 4.7 GPa, and 1.0 to 4 0.7 GPa is more preferable. If the adhesive layer has a breaking strength of 0.1 GPa or more, it is preferable that the adhesive layer is not easily broken when the films are laminated.
- a method of forming a graphite laminate in which a bent portion is formed in advance can be mentioned.
- the graphite laminate by forming a graphite laminate in which a bent portion is formed in advance, the graphite laminate can be connected to a place having a lower temperature, and the heat transport capability can be improved.
- a method for producing a graphite laminate after producing a graphite laminate in which a non-adhered portion in which a part between graphite sheets is not adhered by an adhesive layer is formed, the graphite laminate is not adhered.
- a method of bending at the part can be given.
- a graphite laminated body can hold
- the high temperature part which is a temperature rising part by the heat which a heat source emits the low temperature part which is a part where temperature is lower than a high temperature part, and the connection part with a graphite layered product
- the graphite sheets need to be bonded to each other by the adhesive layer. Therefore, it is preferable that the non-bonded portion is formed at a portion other than both end portions (for example, other than both end portions in the longitudinal direction) of the graphite laminate, which becomes a connection portion to the high temperature portion and the low temperature portion.
- connection part intends the part in a graphite laminated body where the high temperature site
- the method for producing a graphite laminate of the present embodiment is a method for producing a graphite laminate in which graphite sheets and adhesive layers are alternately laminated, and the graphite sheets and adhesive layers are alternately arranged. And laminating to form a laminate, and heating and pressurizing the laminate to adhere the graphite sheet and the adhesive layer to form a graphite laminate.
- the said adhesion process may include the bending part formation process which forms the graphite laminated body which has at least 1 bending part.
- a lamination process is a process of forming a laminate by alternately laminating graphite sheets and adhesive layers.
- a graphite sheet and an adhesive layer having a surface defined by the X axis and a Y axis orthogonal to the X axis intersect perpendicularly with the surface in a state where the surfaces are stacked.
- This is a step of forming a laminate by alternately laminating in the direction of the Z-axis.
- a method of alternately laminating a graphite sheet and a polymer film one by one, and a method of winding a graphite sheet and a polymer film on a core at the same time to form a roll A method of obtaining a laminate of a graphite sheet and a polymer film by cutting and cleaving the roll can be mentioned.
- a graphite adhesive sheet is prepared.
- the graphite adhesive sheet can be produced by applying varnish or laminating an adhesive film.
- the produced graphite adhesive sheet is cut into a single plate and then laminated in multiple layers, and the produced graphite adhesive sheet is used as a core. Examples of the method include forming a roll by winding and then cutting and cleaving the roll.
- Examples of the method for forming the adhesive layer include a method of applying a varnish on a graphite sheet and a method of alternately laminating a film-like adhesive layer and a graphite sheet.
- the method of applying varnish on the graphite sheet it is preferable that the varnish has no tackiness after application from the viewpoint of preventing air from entering the graphite laminate.
- a method of alternately laminating film-like adhesive layers and graphite sheets is adopted, if the dielectric constant of the film-like adhesive layer is low, the film-like adhesive layer is difficult to be charged. It is possible to stably fix the adhesive layer on the conveyor.
- the adhesion step is performed by (i) pressurizing (in other words, compressing), preferably (ii) heating and pressurizing (in other words, compressing) the laminate formed in the laminating step. And a bonding layer to form a graphite laminate.
- bonding process examples include laminating and pressing.
- bonding by pressing is preferable. If it is a press, even a multi-layered laminate of 10 layers or more can be bonded together. Moreover, if pressurization is performed for several seconds or more while heating, the softening of the adhesive layer and the effect of pressurization can suppress air from being caught in the graphite laminate. The contact thermal resistance between them can be reduced.
- the heating temperature and pressurizing pressure are not particularly limited, and can be appropriately selected depending on the material constituting the adhesive layer.
- the laminate formed in the lamination step is heated and pressurized (in other words, compressed).
- the compression ratio of the laminate is not particularly limited, but is preferably smaller than 1, more preferably 0.97 or less, more preferably 0.96 or less, and 0.95 or less. More preferably, it is 0.92 or less, and more preferably 0.90 or less. If the compression ratio (thickness of the graphite laminate / thickness of the laminate as a raw material) is smaller than 1, the adhesive layer is deformed at the time of lamination, so that the graphite sheets easily come into contact with each other, and theoretical heat conduction is achieved. A close graphite stack can be obtained.
- the bent portion may be formed by bending the precursor of the graphite laminate in the process of manufacturing the graphite laminate, or may be formed by bending the graphite laminate after manufacturing the graphite laminate. Good. For example, after a graphite sheet and an adhesive layer are laminated, the laminate is heated and pressurized, and the graphite laminate (in other words, the precursor of the graphite laminate) being formed is bent by the pressurization. Thus, the bent portion may be formed. Or after laminating
- the bent portion forming step forms at least one (for example, one or more, or two or more) bent portions, and forms at least one of the following bent portion forming steps (d) to (h): May contain one: (D) The heated and pressurized laminate is cut in the Z-axis direction, and the graphite laminate is cut out from the laminate, so that the graphite laminate has the X-axis direction or the Y-axis. A first bent portion forming step of forming a first bent portion bent in the axial direction; (E) A second bent portion bent toward the Z-axis direction on the graphite laminate by pressurizing the heated and pressed laminate with a pressurizing jig having a bent shape.
- the graphite laminate After cutting out, by pressing the precursor of the graphite laminate with a bending jig having a bent shape, the graphite laminate is directed toward the X-axis direction or the Y-axis direction.
- a fourth bent portion forming step that forms a third bent portion that is bent and bent toward the Z-axis direction; (H) Pressing the heated and pressurized laminate with a pressure jig having a bent shape to bend the laminate toward the Z-axis, and then By cutting obliquely with respect to the Z-axis direction and cutting out the graphite laminate from the laminate, the graphite laminate is bent toward the X-axis direction or the Y-axis direction, and A fifth bent portion forming step of forming a third bent portion bent in the Z-axis direction.
- the above-described bent portion forming step (e) may be the following bent portion forming step (e ′): (E ′) by pressurizing the heated and pressurized laminate with a pressure jig having a bent shape at two places (in other words, a pressure jig having a bent shape in a stepped manner) , Forming two second bent portions (in other words, two second bent portions bent in opposite directions) bent in the Z-axis direction in the graphite laminate. Bending portion forming step.
- the graphite laminate formed through the above-described bent portion forming step (e) has a shape bent in a step shape (for example, see FIG. 28A).
- the graphite laminate is preferable because it can be disposed in close contact with a structure having a stepped shape and can efficiently carry heat.
- the step height of the graphite laminate having a staircase shape is not particularly limited, but is preferably 0.05 mm to 5.0 mm, more preferably 0.10 mm to 3.0 mm, and most preferably 0.20 mm to 1.0 mm. .
- the bending portion forming step (i) includes the first bending portion forming step and the second bending portion forming step described above when forming a graphite laminate having two or more bending portions.
- the bending portion forming step (i) includes the first bending portion forming step and the second bending portion forming step described above when forming a graphite laminate having two or more bending portions.
- And may include at least one of a third bent portion forming step, a fourth bent portion forming step, and a fifth bent portion forming step, and (ii) a graphite laminate having one or more bent portions.
- the present invention is not limited to these (i) and (ii).
- the two processes (cutting process and pressurizing process) of the bent part forming process described above are processes in which a force that peels off the adhesion between the layers in the laminate is unlikely to occur. Therefore, with the two treatments described above, air can be prevented from entering the graphite laminate, and as a result, a graphite laminate having high thermal conductivity and no voids can be easily obtained. Can be produced.
- FIG. 6 shows an example of the pressurizing process.
- the graphite laminate 1 bent in the direction of the Z-axis at the bent portion 11 is produced by pressing with a pressing jig 30 in which the convex member and the concave member are paired. can do.
- a graphite laminate is cut out using a cutter, a mold, or the like, material loss occurs during cutting.
- it can suppress that the loss of material generate
- Fig. 7 shows an example of the cutting process.
- the graphite laminate 1 bent in the direction of the X axis (or Y axis) at the bent portion 10 is produced by cutting in the Z axis direction along the dotted line 35.
- the cutting process can be performed using a blade saw such as a cutter or outer peripheral blade, a laser, a water jet, a wire saw, etc., but it can prevent delamination of the graphite laminate, cut a large amount at once, and improve productivity. From the viewpoint of improvement, it is preferable to use a wire saw. If it is a cutting process, the graphite laminated body 1 can be bent at a sharp angle (for example, right angle).
- FIG. 8 shows an example in which the cutting process is performed after the pressurizing process.
- a bent portion 11 that is bent in the direction of the Z-axis is formed by applying pressure with a pressing jig (not shown) in which a convex member and a concave member form a pair.
- the graphite laminate 1 bent toward the Z-axis direction at the bent portion 11 can be produced by cutting in the Z-axis direction along the dotted line 35. If it is the said method, a thin graphite laminated body can be obtained. Moreover, the graphite laminated body obtained in this way is excellent in heat transport capability.
- a graphite laminated body can be bent roundly (for example, Preferably, a curvature radius is 8 mm or more).
- a dotted line 35 is set linearly in the direction of the Y-axis.
- the graphite laminate is bent in the direction of the Z-axis. 2 bent portions can be formed (corresponding to the third bent portion forming step).
- a dotted line 35 is a part of the graphite laminate 1 and is set obliquely with respect to the Z-axis direction in a part bent toward the Z-axis direction.
- the angle at which the direction of the Z axis intersects with the dotted line 35 is not limited and can be set to a desired angle.
- the graphite laminate is bent in the X-axis direction or the Y-axis direction, and is bent in the Z-axis direction. Can be formed (corresponding to the fifth bent portion forming step).
- the graphite laminate 1 bent in the direction of the X axis (or Y axis) at the bent portion 10 is produced by the method shown in FIG. 7, and then the bent portion 10 is bent by the method shown in FIG.
- the graphite laminate 1 as shown in FIG. 4 is bent toward the X-axis direction or the Y-axis direction as shown in FIG. 4 and toward the Z-axis direction.
- the bent portion 12 can be formed.
- an unbonded portion in which adjacent graphite sheets are not bonded by an adhesive layer may be formed. If it is the said structure, a graphite laminated body can be bent easily.
- an adhesive layer is not disposed in a portion to be an unbonded portion, an adhesive layer is disposed only in a portion to be an adhesive portion, and the graphite sheet and the adhesive layer are stacked. This is a method of pressurizing the entire surface.
- the portion where the adhesive layer 6 is formed becomes the bonded portion 50, and the portion where the adhesive layer 6 is not formed becomes the unbonded portion 51.
- the graphite laminated body which has can be obtained easily.
- the adhesive layer 6 is not disposed in the non-bonded portion 51, a gap is formed between the graphite sheets 5, and an air flow is generated there. The performance can be improved. Further, since the adhesive layer 6 is not formed on the unbonded portion 51, the flexibility of the bent portion is improved.
- the adhesive layer is arranged on the entire surface of the graphite sheet and laminated, and then a part of the laminate is pressurized (preferably, a part of the laminate is heated and pressurized).
- a part of the laminate is heated and pressurized.
- the bonded portion and the non-bonded portion can be formed by pressing only the portion to be the bonded portion with a jig (preferably, only the portion to be the bonded portion is pressed with a jig while heating).
- a graphite laminate having the following can be obtained.
- the graphite sheet 5 is not adhere
- the part shown with the dotted line of the non-bonding part 51 of FIG. 10 has shown the location where the graphite sheet 5 and the contact bonding layer 6 are not adhere
- the heat transport structure of the present embodiment is a heat transport structure including the graphite laminate of the present invention and a heating element, and the graphite stack is emitted by the heating element. It is connected to a high-temperature part that is a part that is heated by heat and a low-temperature part that is a part that is lower in temperature than the high-temperature part.
- a high-temperature portion that is a portion that is heated by heat generated by the heating element refers to a portion that is affected by the heat generated by the heating element.
- the heating element 100 may be disposed so as to be in contact with the graphite laminate 1.
- FIG. 11 shows a composite body of the heating element 100 and the graphite laminate 1 in a side view 110 and a top view 120.
- the surface of the heat generating element 100 or the vicinity thereof, and the surface of the heat generating element 100 in contact with the graphite laminate 1 or the vicinity thereof is a “high-temperature part that is a part that is heated by heat generated by the heat generating element”. included. It is possible to arrange other configurations or a hollow space between the heating element 100 and the graphite laminate 100.
- the “neighborhood” described above may include other configurations and hollow spaces.
- the location where the heat generating element comes into contact and the vicinity thereof are also included in the “high temperature portion where the temperature is increased by the heat generated by the heat generating element” as long as the portion is affected by the heat generated by the heat generating element.
- the metal plate 101 may be disposed on the graphite laminate 1, and the heating element 100 may be disposed so as to be in contact with the metal plate 101.
- the surface of the metal plate 101 or the vicinity thereof and the surface in contact with the heating element 100 And the vicinity thereof are included in “a high-temperature portion that is a portion that is heated by heat generated by the heating element”.
- a metal which comprises the metal plate 101 For example, copper, aluminum, nickel, etc. can be mentioned.
- a high-temperature part that is a part that is heated by heat generated by the heat generating element as long as it is a part that is affected by the heat generated by the heat generating element even if the part is not in contact with the heat generating element or the vicinity thereof. That is, the “high temperature part, which is a part where the temperature is raised by the heat generated by the heat generating element”, is not limited to the place where the heat generating element is in contact or the vicinity thereof, and is not limited to the part where heat generated by the heat generating element is concentrated. As shown in FIG.
- a metal plate 101 is disposed on the graphite laminate 1, and a heat transfer material 102 (for example, a metal such as a graphite sheet or copper, a heat pipe) is disposed on the metal plate 101 to generate heat.
- the element 100 may be disposed in contact with the heat transfer material 102.
- the surface of the metal plate 101 and the vicinity thereof, and the surface and the vicinity thereof that are affected by the heat generated by the heat generating element 100 are included in the “high temperature part that is a part that is heated by heat generated by the heat generating element” It is.
- the low temperature part is a part having a temperature lower than the above-described high temperature part.
- the specific configuration is not particularly limited, and may be any part as long as the temperature is lower than the high temperature part.
- the heat transport structure of the present embodiment can diffuse the heat generated by the heating element over a wide range by utilizing the high thermal conductivity of the graphite laminate of the present invention. Furthermore, the heat transport structure of the present embodiment uses the graphite laminate of the present invention, which is a laminate, so that the amount of heat that can be transported at one time is large. High effect.
- the laminated surface 7 means a surface formed by exposing the surface of the graphite laminate 1 in a state where the graphite sheet 5 and the adhesive layer 6 are arranged in stripes.
- a surface extending in the YZ plane is shown as a laminated surface, but a surface extending in the XZ plane can also be included in the laminated surface.
- the graphite sheet has a thermal conductivity in the thickness direction of 5 W / (m ⁇ K), and the thermal conductivity in the thickness direction is lower than the thermal conductivity in the plane direction.
- the thermal conductivity in the lamination direction is 5 W. / (M ⁇ K) or less.
- the graphite sheets are laminated in multiple layers, and since the thickness in the lamination direction is large, the heat generated by the heating element is also sufficient to the surface opposite to the heat receiving surface of the graphite laminate. Therefore, it is important to transfer the heat to the low temperature part by using the entire graphite laminate efficiently.
- the graphite sheet has a high thermal conductivity of 1500 W / (m ⁇ K) in the plane direction, the opposite side of the heat receiving surface of the graphite laminate is obtained by making the laminate surface of the graphite laminate face the high temperature portion. It is good because the heat can be sufficiently transferred to the surface of the film, and the entire graphite laminate can be efficiently used and transferred to a low temperature region.
- the length of the graphite laminate in the lamination direction is a short side of the surface perpendicular to the lamination direction of the graphite laminate (the shape of the surface is, for example, a rectangle). It is preferable that the length is longer than the length. More specifically, in FIGS. 15 and 16, the length of the graphite laminate 1 in the Z-axis direction is preferably thicker than the length of the graphite laminate 1 in the X-axis direction.
- the length of the graphite laminate in the lamination direction is preferably 2 mm or more, and more preferably 2.5 mm or more.
- the bent portion is provided in the graphite laminate 1 as shown in FIG. 16, as in the case where the surface of the graphite laminate is opposed to the high temperature portion.
- the heat receiving efficiency of the graphite laminated body 1 is further improved, and the bent part is further provided to connect the graphite laminated body 1 to the low temperature part having a lower temperature.
- the high heat transport capability of the heat transport structure can be realized.
- FIG. 17 and FIG. 18 show examples of the dimensions of the graphite laminate, but the present invention is not limited to these configurations.
- the present invention can also be configured as follows.
- a graphite laminate in which a plurality of graphite sheets and adhesive layers are alternately laminated The adhesive layer includes a thermoplastic resin and / or a thermosetting resin, The adhesive layer has a water absorption of 2% or less and a thickness of less than 10 ⁇ m, The graphite laminate, wherein the number of laminated graphite sheets is 5 or more.
- a graphite laminate in which a plurality of graphite sheets and adhesive layers are alternately laminated The adhesive layer includes a thermoplastic resin and / or a thermosetting resin, The adhesive layer has a water absorption of 2% or less, The thickness of the graphite laminate is smaller than the sum of the thickness of the raw material sheet of the graphite sheet and the thickness of the adhesive layer, The graphite laminate, wherein the number of laminated graphite sheets is 5 or more.
- ⁇ 4> The graphite laminate according to any one of ⁇ 1> to ⁇ 3>, wherein the thermal conductivity in the plane direction of the graphite sheet is 1000 W / (m ⁇ K) or more.
- a value (Tg / Ta) obtained by dividing the total thickness (Tg) of each graphite sheet by the total thickness (Ta) of each of the adhesive layers is 4.1 or more and 40 or less,
- the length of the graphite laminate in the lamination direction is 0.5 mm or more, according to any one of ⁇ 1> to ⁇ 4>, Graphite laminate.
- ⁇ 6> Specified by a plane (specifically, an X axis and a Y axis intersecting the X axis) perpendicular to the stacking direction (specifically, the direction of the Z axis) of the graphite laminate.
- At least one of the bent portions is a direction (specifically, an X-axis direction or a Y-axis direction) perpendicular to the stacking direction (specifically, the Z-axis direction) of the graphite laminate.
- At least one of the bent portions is a direction (specifically, an X-axis direction or a Y-axis direction) perpendicular to the stacking direction (specifically, the Z-axis direction) of the graphite laminate.
- the graphite laminate has an unbonded portion where the graphite sheets are not bonded to each other by the adhesive layer,
- the length in the stacking direction (specifically, the direction of the Z axis) is perpendicular to the stacking direction (specifically, the X axis and the Y axis intersecting the X axis).
- a structure comprising the graphite laminate according to any one of the above ⁇ 1> to ⁇ 16>, and a heating element, One end of the graphite laminate is disposed at a high temperature site that is a temperature raised by heat generated by the heating element, The other end of the graphite laminate is disposed in a low-temperature part, which is a part having a temperature lower than that of the high-temperature part.
- a laminate surface of the graphite laminate (specifically, a surface of the graphite laminate parallel to the Z-axis direction) is disposed so as to face the high temperature portion.
- a lamination step of alternately laminating graphite sheets and adhesive layers comprising: an adhesion step in which each layer is adhered by heating and pressing.
- the adhesive layer expresses adhesiveness by heating, In the said adhesion process, each layer is adhere
- the graphite laminate is bent in the stacking direction of the graphite stack (specifically, the Z-axis direction) by pressing with a pressure jig having a bent shape.
- the graphite laminate is cut in the lamination direction (specifically, the Z-axis direction) to cut out the graphite laminate, ⁇ 19> to ⁇ 21>
- the manufacturing method of the graphite laminated body in any one of.
- the graphite laminate is bent in the stacking direction of the graphite laminate (specifically, the Z-axis direction) by applying pressure with a pressure jig having a bent shape. Then, the method for producing a graphite laminate according to any one of ⁇ 19> to ⁇ 21>, wherein the graphite laminate is cut in a lamination direction (specifically, a Z-axis direction).
- the present invention can be configured as follows.
- the graphite laminate of the present invention is a graphite laminate in which graphite sheets and adhesive layers are alternately laminated, and the adhesive layer includes at least one of a thermoplastic resin and a thermosetting resin.
- the adhesive layer has a water absorption of 2% or less, and the graphite laminate is obtained by compressing a laminate in which the graphite sheet and the adhesive layer are alternately laminated.
- the number of the graphite sheets included in the graphite laminate is 3 or more (or 5 or more).
- the graphite laminate of the present embodiment is a graphite laminate including graphite sheets and adhesive layers that are alternately laminated (or a graphite laminate in which graphite sheets and adhesive layers are alternately laminated).
- the adhesive layer material which is the material of the adhesive layer, or the adhesive layer contains at least one of a thermoplastic resin and a thermosetting resin.
- the number of graphite sheets included in the graphite laminate is three or more.
- the graphite laminate is obtained by heating and pressing a laminate in which graphite sheets and adhesive layer materials are alternately laminated.
- the graphite laminate of the present invention may have a shape bent at at least one bent portion of the graphite laminate.
- This graphite laminate may be formed by bending a laminate, or may be formed by bending a graphite laminate.
- C-1-1. (Graphite laminate) (Basic structure of graphite laminate)
- the graphite laminate is formed by alternately laminating graphite sheets and adhesive layers.
- another structure may be inserted
- FIG. 20 is a diagram showing a basic structure of a graphite laminate.
- each of the graphite sheet 205 and the adhesive layer 206 constituting the graphite laminate 201 has a surface defined by the X axis and a Y axis perpendicular to the X axis. Then, in a state where the surfaces overlap, the graphite sheets 205 and the adhesive layers 206 are alternately stacked in the direction of the Z axis perpendicular to the surfaces, thereby forming the graphite laminate 201. Yes. As described above, the angle at which the X axis and the Y axis intersect is 90 °.
- the graphite sheet and the adhesive layer are in close contact with each other (for example, heat fusion) at 50% or more of the interface.
- the graphite sheet and the adhesive layer are preferably in close contact at 70% or more of the interface, and more preferably at 80% or more of the interface, from the viewpoint of adhesive thermal resistance (easy heat transfer). Further, it is more preferable that the contact is made at 95% or more of the interface. Since the ease of heat transfer has been described in the examples described later, the description thereof is omitted here.
- the surface is overlapped means that at least a part of the graphite sheet 205 and at least a part of the adhesive layer 206 overlap when the laminate 201 is viewed from the Z-axis direction in FIG. Refers to the state of being.
- the graphite sheet 205 and the adhesive layer 206 may be the same or different in shape and size. From the standpoint of realizing the desired effect better, it is preferable that the shape of the graphite sheet 205 and the adhesive layer 206 have the same shape and size.
- the shape of the graphite sheet 205 and the shape of the adhesive layer 206 may be square.
- the direction in which one side of the square extends can be the X-axis direction
- the direction in which another side that intersects the side extends can be the Y-axis direction.
- the shape of the graphite sheet 205 and the shape of the adhesive layer 206 may be rectangular.
- the direction in which the short side of the rectangle extends can be the X-axis direction
- the direction in which the long side of the rectangle extends can be the Y-axis direction.
- the graphite sheet 205 and the adhesive layer 206 may have a shape other than a square or a rectangle.
- the most longitudinal direction of the graphite sheet 205 and the adhesive layer 206 can be the Y-axis direction, and the direction orthogonal to the Y-axis can be the X-axis direction.
- the number of graphite sheets contained in the graphite laminate may be 3 or more, but from the viewpoint of heat capacity, it is more preferably 5 or more, more preferably 10 or more, and 15 or more. More preferably, there are more than 20 layers.
- the upper limit of the number of stacked layers is not particularly limited, and may be 1000 layers or less, 500 layers or less, 200 layers or less, 100 layers or less, 80 layers or less, or 50 layers or less.
- the number of laminated graphite sheets is 3 or more because a graphite laminate having high heat transport capability and excellent mechanical strength can be obtained.
- the number of adhesion layers included in the graphite laminate is not particularly limited, and can be appropriately set according to the number of graphite sheets.
- two or more adhesive layers as well as one adhesive layer may be disposed between adjacent graphite sheets.
- It may be disposed only on the top surface of the body, only on the bottom surface of the graphite laminate, or may be disposed on both the top surface and the bottom surface of the graphite laminate. It may be disposed only on the uppermost surface, disposed only on the lowermost surface of the graphite laminate, or may be disposed on both the uppermost surface and the lowermost surface of the graphite laminate.
- graphite sheets and adhesive layers are alternately laminated includes (a) a case where one adhesive layer is disposed between adjacent graphite sheets, and (b) adjacent graphite sheets. Both are included when two or more adhesive layers are disposed between them. That is, in the present invention, the adhesive layer may be a laminate of a plurality of adhesive layers.
- the thickness of the graphite laminate (in other words, the length in the Z-axis direction in FIG. 20) is not particularly limited, and is preferably 0.1 mm or more, more preferably 0.4 mm or more, and 0 More preferably, it is 6 mm or more, and more preferably 0.8 mm or more. If the thickness of the graphite laminate is 0.1 mm or more, the amount of heat that can be transported increases, and the present invention can also be applied to electronic devices that generate a large amount of heat.
- the upper limit value of the thickness of the graphite laminate is not particularly limited, and may be 10 mm or less, 7.5 mm or less, or 5 mm or less from the viewpoint of thinning the electronic device. Alternatively, it may be 2.5 mm or less, or 1 mm or less.
- lamination via an adhesive layer is effective in order to absorb irregularities on the surface of the graphite sheets and reduce contact thermal resistance between the graphite sheets.
- the graphite laminate may have a shape bent at at least one (for example, one or more, or two or more) bent portions provided in the graphite laminate.
- the graphite laminate can be obtained by bending the graphite laminate before bending at the bent portion.
- the low temperature part and the heat source cannot always be connected linearly. Therefore, by forming a bent portion in the graphite laminate, the heat generated by the heat source can be moved to a lower temperature portion, thereby further improving the heat transport capability. That is, the degree of freedom in the arrangement relationship between the heat source and the lower temperature portion can be increased.
- the configuration of the bent portion described in the embodiment B can be employed.
- the angle at which the bent part bends is not particularly limited.
- the bent portion may be bent with a curvature radius of 2 mm or more, a curvature radius of 5 mm or more, a curvature radius of 8 mm or more, a curvature radius of 10 mm or more, or a curvature radius of 20 mm or more.
- the maximum value of the radius of curvature is not particularly limited, and may be, for example, 100 mm, 90 mm, 80 mm, 70 mm, 60 mm, 50 mm, 40 mm, 30 mm, or 20 mm. Of course, the maximum value of the radius of curvature may be a value larger than 100 mm.
- the graphite composite product is obtained by bonding a sheet having at least an adhesive or an adhesive to at least one surface of a graphite laminate.
- a graphite laminate for heat transportation can be attached to a semiconductor element or other heat generating component mounted on various electronic / electrical devices such as a computer.
- the structure of the sheet having the adhesive material is not particularly limited.
- the sheet made of the adhesive material the sheet including the two-layer structure of the adhesive material / base material, and the sheet including the three-layer structure of the adhesive material / base material / adhesive material.
- the adhesive material is not particularly limited, and a silicone-based adhesive material, an acrylic adhesive material, a synthetic rubber-based adhesive material, or the like can be used.
- the substrate is not particularly limited, and is not limited to polyimide resin, polyethylene terephthalate (PET) resin, polyphenylene sulfide (PPS) resin, polyethylene naphthalate (PEN) resin, polyester resin, or metal sheet (for example, Aluminum foil, copper foil, etc.) can be used.
- the structure of the sheet having an adhesive is not particularly limited, and for example, a film made of an adhesive, a sheet including a two-layer structure of adhesive / base, and a sheet including a three-layer structure of adhesive / base / adhesive And so on.
- the adhesive is not particularly limited, and a thermosetting resin adhesive such as polyimide or epoxy can be used.
- a thermoplastic resin that is bonded in a molten state can also be used.
- the substrate is not particularly limited, and is not limited to polyimide resin, polyethylene terephthalate (PET) resin, polyphenylene sulfide (PPS) resin, polyethylene naphthalate (PEN) resin, polyester resin, metal sheet (for example, aluminum foil) , Copper foil, etc.), CFRP (carbon fiber reinforced material), carbon fiber felt, or other carbon materials.
- PET polyethylene terephthalate
- PPS polyphenylene sulfide
- PEN polyethylene naphthalate
- polyester resin polyester resin
- metal sheet for example, aluminum foil
- CFRP carbon fiber reinforced material
- carbon fiber felt or other carbon materials.
- the above-described graphite laminate and graphite composite of the present invention can be used for a heat transport structure mainly as a heat transport material for electronic equipment.
- the structure for heat transport includes a graphite laminate or a graphite composite article and a heating element, and the graphite laminate or the graphite composite article has a high temperature part that is heated by heat generated by the heating element and a high temperature part. It is connected to a low temperature part that is a part having a lower temperature than the part.
- thermo conductivity in the surface direction of the graphite sheet Regarding the thermal conductivity in the surface direction of the graphite sheet of [Embodiment C], the same configuration as that described in the column of (thermal conductivity in the surface direction of the graphite sheet) in [Embodiment B] should be adopted. Can do.
- the thermal conductivity in the plane direction of the graphite sheet was calculated by the following equation (1).
- A ⁇ ⁇ d ⁇ Cp (1)
- A the thermal conductivity of the graphite sheet
- ⁇ the thermal diffusivity of the graphite sheet
- d the density of the graphite sheet
- Cp the specific heat capacity of the graphite sheet.
- the thermal diffusivity of the graphite sheet is measured using a thermal diffusivity measuring device based on the optical alternating current method (for example, “LaserPit” manufactured by ULVAC-RIKO Co., Ltd.). The measurement was performed under an alternating current condition of 10 Hz in an atmosphere of 20 ° C.
- Adhesive layer (Type of adhesive layer material)
- the adhesive layer material that is the material of the adhesive layer in the present invention is preferably one that exhibits adhesiveness by heating, and a thermosetting resin or a thermoplastic resin can be used.
- thermosetting resin the same thermosetting resin as described in the column of (Type of adhesive layer) in [Embodiment B] can be used.
- thermoplastic resin the same thermoplastic resin as described in the column of (Type of adhesive layer) in [Embodiment B] can be used.
- the adhesive layer material it is preferable to use an aromatic material (eg, polyester adhesive, polyethylene terephthalate, etc.).
- aromatic material eg, polyester adhesive, polyethylene terephthalate, etc.
- the thermoplastic resin and the thermosetting resin preferably have a melting temperature of 50 ° C. or higher, more preferably 60 ° C. or higher, more preferably 70 ° C. or higher, and 80 ° C.
- the above is more preferable. If the melting temperature is 50 ° C. or higher, air can be better prevented from entering the graphite laminate.
- the melting temperature of the adhesive layer material can be measured by a differential scanning calorimeter (DSC-50 manufactured by Shimadzu Corporation) in accordance with JIS K7121.
- the elastic modulus of the adhesive layer material is not particularly limited, but is preferably high (for example, the elastic modulus is 100 MPa or more) from the viewpoint of suppressing variations in the thickness of the adhesive layer when the graphite laminate is cut.
- the thickness of the adhesive layer material in the present invention is not particularly limited, and is preferably less than 10 ⁇ m. More specifically, the thickness of the adhesive layer material is preferably 0.1 to 10 ⁇ m, more preferably 1 to 10 ⁇ m, more preferably 1 to 9 ⁇ m, and more preferably 1 to 7 ⁇ m. If the thickness of the adhesive layer material is less than 10 ⁇ m, the thermal conductivity of the adhesive layer is much smaller than that of the graphite sheet. Therefore, by controlling the thickness of the adhesive layer material to be less than 10 ⁇ m, heat can be transferred favorably without hindering heat transfer between the graphite sheets by the adhesive layer.
- the thickness of the adhesive layer material is 0.1 ⁇ m or more (more preferably, 1 ⁇ m or more), the adhesive layer easily absorbs irregularities on the surface of the graphite sheet, and the contact thermal resistance between the graphite sheet and the adhesive layer is reduced. Heat can be transferred efficiently. Moreover, if the thickness of the adhesive layer material is 0.1 ⁇ m or more (more preferably, 1 ⁇ m or more), the adhesive layer can exhibit good adhesiveness. Moreover, if it is the thickness of the contact bonding layer material mentioned above, the thermal conductivity of a graphite laminated body can be made into the value close
- the thickness of the adhesive layer in the present invention is the same as or thinner than the thickness of the adhesive layer material. When the adhesive layer is thinner than the adhesive layer material, it is considered that the adhesive layer material has infiltrated the surface of the graphite sheet (absorbs the irregularities on the surface of the graphite sheet).
- the specific thickness of the adhesive layer is not particularly limited, and is preferably less than 10 ⁇ m. More specifically, the thickness of the adhesive layer is preferably from 0.1 ⁇ m to less than 10 ⁇ m, more preferably from 1 ⁇ m to less than 10 ⁇ m, more preferably from 1 ⁇ m to 9 ⁇ m, and more preferably from 1 ⁇ m to 7 ⁇ m.
- the thermal conductivity of the adhesive layer is much smaller than that of the graphite sheet. Therefore, by controlling the thickness of the adhesive layer to be less than 10 ⁇ m, it is possible to transfer heat well without inhibiting the heat transfer between the graphite sheets by the adhesive layer. If the thickness of the adhesive layer is 0.1 ⁇ m or more (more preferably 1 ⁇ m or more), the adhesive layer easily absorbs irregularities on the surface of the graphite sheet, and the contact thermal resistance between the graphite sheet and the adhesive layer is reduced. Can transfer heat efficiently. Moreover, if the adhesive layer is 0.1 ⁇ m or more (more preferably 1 ⁇ m or more), good adhesiveness can be exhibited. Moreover, if it is the thickness of the contact bonding layer mentioned above, the thermal conductivity of a graphite laminated body can be made into the value close
- the method described later can be mentioned. Specifically, the cross section of an arbitrary adhesive layer is observed with an SEM image, the thickness of the adhesive layer at any nine points is measured, The average value of the measured values may be calculated as the thickness of the adhesive layer.
- the method for producing a graphite laminate of the present invention includes a lamination step in which a graphite sheet and an adhesive layer material are alternately laminated to form a laminate, and the graphite sheet and the adhesive layer are thermally fused by heating the laminate. Adhering step to form a graphite laminate by attaching. Furthermore, the manufacturing method of a graphite laminated body may have the cutting process of cutting-processing a graphite laminated body.
- the term “heat fusion” means that the resin or wax is softened by heating and adheres to another substance.
- the laminating step is a step of forming a laminate by alternately laminating a plurality of adhesive layer materials, which are materials of the adhesive layer, and graphite sheets.
- the laminating step is a process of stacking a graphite sheet and an adhesive layer material having a surface defined by an X axis and a Y axis orthogonal to the X axis, with the surfaces overlapped, perpendicular to the upper surface. It is a step of forming a laminate by alternately laminating in the direction of the intersecting Z-axis.
- a graphite adhesive sheet is prepared.
- the graphite adhesive sheet can be produced by applying an adhesive layer material (for example, an adhesive resin sheet) to the graphite sheet or laminating an adhesive layer material (for example, an adhesive film).
- an adhesive layer material for example, an adhesive resin sheet
- laminating an adhesive layer material for example, an adhesive film
- the produced graphite adhesive sheet is cut into a single plate, and then the graphite adhesive sheet is laminated in multiple layers, and the produced graphite adhesive sheet is used as a core. Examples thereof include a method of cutting and cleaving the roll after it is wound to form a roll.
- the adhesive layer material When the adhesive layer material is applied on the graphite sheet, the adhesive layer material preferably has no tackiness after application from the viewpoint of preventing air from entering the graphite laminate.
- the adhesive layer material and the graphite sheet are alternately laminated, or when the adhesive layer material is laminated on the graphite sheet, if the adhesive layer material has a low dielectric constant, the adhesive layer material is difficult to be charged.
- the adhesive layer material can be stably fixed to the conveyor.
- the electrical conductivity of the graphite sheet is high, when the graphite sheet and the adhesive layer material are in close contact, static electricity of the adhesive layer material escapes to the graphite sheet, and the slip between the graphite sheet and the adhesive layer material is improved. The wrinkles of the adhesive layer material are less likely to occur.
- the lamination process it is preferable to laminate a plurality of laminates from the viewpoint that the graphite laminates can be peeled off after heat fusion and a plurality of graphite laminates can be produced simultaneously.
- the number of stacked layers of the laminate is preferably 100 or more, more preferably 200 or more from the viewpoint of mass productivity.
- the upper limit of the number of stacked layers of the laminate is not particularly limited, and may be, for example, 1000, 900, 800, 700, 600, 500, 400, or 300.
- the adhesion ratio value is good for any graphite laminate in which the lamination position in one batch is the upper part, the middle part, and the lower part. It becomes.
- the bonding step is a step of heating the laminate formed in the laminating step to thermally fuse the adhesive layer material to the graphite sheet to obtain a graphite laminate in which the adhesive layer and the graphite sheet are alternately laminated. It is.
- the heating temperature is not particularly limited and can be appropriately selected depending on the adhesive layer material.
- first pressurization and second pressurization are performed.
- the two-stage pressurization of the first pressurization and the second pressurization causes the gas in the laminate to escape well, so that a graphite laminate having high smoothness and high peel strength can be obtained.
- the heating temperature, the first pressurizing pressure, and the second pressurizing pressure are not particularly limited, and can be appropriately selected according to the adhesive layer material.
- pressurization such as the third pressurization and the fourth pressurization may be further performed once or more. Further, in the bonding step, the pressurization such as the third pressurization and the fourth pressurization may be further performed once or more between the first pressurization and the second pressurization.
- one or more preliminary pressurizations may be performed before the first pressurization. However, the pressure applied to the laminate by the pre-pressurization is lower than the pressure applied to the laminate by the first pressurization and the pressure applied to the laminate by the second pressurization. It is preferable. If it is the said structure, the gas in a laminated body will escape still better. Note that the third pressurization, the fourth pressurization, and the pre-pressurization can be performed in steps other than the bonding step.
- the first pressurization means to pressurize the laminate at least until the temperature of the heated adhesive layer material reaches [(melting temperature of adhesive layer material) ⁇ 20 ° C.].
- [(Melting temperature of adhesive layer material) ⁇ 20 ° C.] means that the temperature of the adhesive layer material is measured in a state where a thermocouple is in contact with the laminate, and the measured temperature is 20 ° C. lower than the melting of the adhesive layer material. When the temperature is reached. In other words, in the present embodiment, the temperature of the adhesive layer material is measured in a state where the laminate is in contact with the thermocouple, and until the measured temperature reaches 20 ° C. lower than the melting of the adhesive layer material, One pressurization may be performed.
- the first pressurization is not particularly limited as long as the pressure is such that the adhesive layer material is not thermally fused to the graphite sheet, and can be appropriately selected according to the adhesive layer material.
- the first pressurization time is not particularly limited, but it is preferable to perform the first pressurization from the start of the adhering step because a graphite laminate having higher smoothness and peel strength can be obtained.
- the second pressurization means to pressurize at least the laminate after the temperature of the heated adhesive layer material becomes [(melting temperature of adhesive layer material) ⁇ 20 ° C.] or higher.
- “After [(melting temperature of adhesive layer material) ⁇ 20 ° C.]” means that the temperature of the adhesive layer material is measured in a state where a thermocouple is in contact with the laminate, and the measured temperature is [(adhesion The melting temperature of the layer material) -20 ° C.] or later. That is, in the present embodiment, when the temperature of the adhesive layer material is measured in a state where the laminate is in contact with the thermocouple, and the measured temperature becomes [(melting temperature of the adhesive layer material) ⁇ 20 ° C.] or higher.
- the second pressurization is not particularly limited as long as the pressure is such that the adhesive layer material is thermally fused to the graphite sheet, and can be appropriately selected according to the adhesive layer material.
- the second pressurization time is not particularly limited, but is preferably 1 minute or more and 10 minutes or less, more preferably 3 minutes or more and 8 minutes or less, and more preferably 4 minutes or more from the viewpoint of improving the adhesion between the graphite sheet and the adhesive layer. 6 minutes or less is particularly preferable.
- the second pressurization is performed continuously after the first pressurization.
- the second pressurization may pressurize the laminate at a higher pressure than the first pressurization, and (ii) the second pressurization is more than the first pressurization.
- the laminate may be pressurized at a high pressure and a high temperature.
- the pressure applied to the laminate may be gradually increased. In the pressure, the pressure applied to the laminate may be gradually increased.
- V In the first pressurization, the pressure applied to the laminate is gradually increased, and then the second pressurization is performed. The pressure applied to the object may be gradually increased.
- the adhesive layer is deformed to match the shape of the irregularities on the surface of the graphite sheet by sequentially increasing the pressure applied to the laminate. Since the timing to perform and the timing to deform the graphite sheet can be adjusted, the adhesive strength between the graphite sheet and the adhesive layer can be improved.
- the bonding process include laminating and pressing.
- bonding by pressing is preferable. If it is a press, even if it is a multilayer laminate of 10 layers or more, each layer in the laminate can be bonded together.
- the laminate is heated for several seconds or more while the laminate is heated, air can be prevented from being caught in the graphite laminate due to the softening of the adhesive layer and the effect of the pressurization. Thereby, the contact thermal resistance between graphite sheets can be reduced.
- the laminate formed in the lamination step is heated and pressurized (in other words, compressed).
- the compression ratio of the laminate is not particularly limited, and is preferably less than 1, more preferably 0.97 or less, more preferably 0.96 or less, and 0.95 or less. More preferably, it is 0.92 or less, and more preferably 0.90 or less. If the compression ratio (thickness of the graphite laminate / thickness of the laminate as a raw material) is less than 1, the laminated adhesive layer is deformed, so that the graphite sheets are easily brought into contact with each other and are close to theoretical heat conduction. A graphite laminate can be obtained.
- FIG. 21 shows an example of the cutting process.
- the stacked body 201 can be manufactured.
- the cutting process can be performed using a blade saw such as a cutter or outer peripheral blade, a laser, a water jet, a wire saw, etc., but it can prevent delamination of the graphite laminate, cut a large amount at once, and improve productivity. From the viewpoint of improvement, it is preferable to use a wire saw. If it is a cutting process, the graphite laminated body 201 can be bent at a sharp angle (for example, right angle).
- the graphite laminate described in Embodiment A to Embodiment C can also be configured as a graphite composite film including a graphite laminate, a protective layer, and an adhesive layer.
- the graphite composite film is a graphite composite film composed of a graphite laminate, a protective layer, and an adhesive layer, and at least a part of the end of the graphite laminate is covered with the protective layer and the adhesive layer. Preferably it is.
- the graphite composite film can be configured according to Japanese Patent Publication “JP 2008-80672 (published Apr. 10, 2008)”.
- JP 2008-80672 published Apr. 10, 2008
- the Japanese published patent publication is incorporated herein by reference.
- Below, a graphite composite film is demonstrated concretely.
- the graphite composite film it is preferable that at least a part of the end of the graphite laminate is covered with a protective layer and an adhesive layer. More specifically, the graphite composite film includes (i) a structure in which all ends of the graphite laminate are covered with a protective layer and an adhesive layer, and (ii) a part of the ends of the graphite laminate is adhered to the protective layer. It may have a structure coated with a layer, or (iii) a structure in which the entire graphite laminate is coated with a protective layer and an adhesive layer.
- a graphite composite film in which at least a part of the end of the graphite laminate is covered with a protective layer and an adhesive layer the graphite composite film is agglomerated and broken between the graphite layers when the graphite composite film is peeled off from the release liner or reworked. It becomes possible to prevent this. Furthermore, in small electronic devices such as mobile phones, notebook PCs, handy camcorders, and automobile headlamps, the space inside the devices is reduced, resulting in a reduction in heat radiation space. For this reason, cases where the heat transport film is attached to a movable part such as a hinge part or a flexible substrate, or the heat transport film is curved in the apparatus are rapidly increasing.
- the graphite composite film of the present invention may cause delamination from the end, or the interface between the protective layer and the graphite laminate or the adhesive layer. It becomes a heat transport film that can withstand bending and repeated bending without causing interface peeling from the interface of the graphite film.
- ⁇ Projection width of protective layer> When the peripheral edge part of a graphite laminated body is coat
- the protruding width of the protective layer is 2 mm or less, preferably 1 mm or less. If the protrusion width is 2 mm or less, the protruding portion that does not contribute to the thermal diffusion around the graphite laminate can be reduced, and in a space-saving electronic device, the area of the graphite laminate can be increased, and the heat dissipation characteristics are excellent. An electronic device can be realized.
- the ratio of the protruding area defined by (area of protective layer ⁇ area of graphite laminate) / (area of graphite laminate) is 50% or less, preferably 30% or less, more preferably 10% or less. If the ratio of the protruding area is 50% or less, the protruding portion that does not contribute to the thermal diffusion around the graphite laminate can be reduced, and in a space-saving electronic device, the area of the graphite laminate can be designed to be large, and the heat dissipation characteristics It is possible to realize an excellent electronic device.
- the coating ratio defined by (length at which the end of the graphite laminate is covered) / (end length of the graphite laminate) is 10% or more, preferably 20% or more, more preferably 30% or more. . If the graphite composite film is a graphite composite film in which at least a part of the end of the graphite laminate is coated with a protective layer and an adhesive layer at a coating ratio of 10% or more, the graphite composite film is peeled off from the release liner or reworked. It becomes possible to prevent cohesive failure between graphite layers.
- the graphite composite film is used in a bent state or repeatedly bent state, delamination occurs from the edge of the graphite composite film, or interfacial delamination occurs from the interface between the protective layer or adhesive layer and the graphite laminate.
- the film for heat transport can withstand bending and repeated bending.
- the thickness of the graphite composite film is 100 ⁇ m or less, preferably 90 ⁇ m, and more preferably 80 ⁇ m or less. If it is a graphite composite film with a thickness of 100 ⁇ m or less, the graphite composite film was peeled off, reworked, or used for bending and repeated bending, and bending force was applied to the graphite composite film with a steep curvature. Even in such a case, it becomes difficult to apply an extra force to the graphite layer, and the delamination of the graphite hardly occurs.
- the thermal conductivity of the graphite composite film is 400 W / m ⁇ K or more, preferably 500 W / m ⁇ K or more, and more preferably 600 W / m ⁇ K or more.
- the thermal conductivity is 400 W / m ⁇ K or higher, the heat conductivity is high, so that heat is easily released from the heat generating device, and the temperature rise of the heat generating device can be suppressed.
- the thermal conductivity mentioned here is a value calculated from the product of thermal diffusivity, heat capacity, and density.
- the MIT (R1mm) of the graphite composite film is 100,000 times or more, preferably 200,000 times or more, more preferably 300,000 times or more.
- the graphite composite film can be suitably used as a hinge of a mobile phone or a bent portion of a small electronic device.
- the bending angle can be selected, and R can be selected to be 5 mm, 2 mm, 1 mm, or the like.
- excellent bendability at R1 mm is very important because it enables a space-saving design of the device.
- the measurement method of MIT (R1 mm) may be according to the measurement method described in Japanese Patent Publication “Japanese Patent Laid-Open No. 2008-80672 (published Apr. 10, 2008)”.
- the protective layer protects the surface from scratches and wrinkles when the graphite laminate is handled or attached to an electronic device.
- Graphite powder may peel off from the surface of graphite, and a protective layer is formed to prevent the powder from falling off.
- the adhesive layer can be used to adhere the graphite laminate to the heat generating component, the heat radiating component, or the housing.
- the thickness of each of the protective layer and the adhesive layer is 40 ⁇ m or less, preferably 30 ⁇ m or less, and more preferably 20 ⁇ m or less.
- a protective layer and an adhesive layer having a thickness of 40 ⁇ m or less are used for the protective layer and the adhesive layer, respectively, the graphite composite film can be peeled off, reworked, used for bending and repeated bending, and the like. Even when a bending force is applied with a steep curvature, it is difficult for an extra force to be applied to the graphite layer, and film delamination hardly occurs.
- the protective layer include an insulating layer and a conductive layer.
- the material for the insulating layer include polyimide, polyethylene terephthalate, and epoxy. These materials have excellent heat resistance, and are sufficient even when a graphite composite film is used in combination with a heat-generating component or a heat-dissipating component. Long-term reliability.
- the thickness of the insulating layer is 40 ⁇ m or less, preferably 30 ⁇ m or less, more preferably 20 ⁇ m or less. When the thickness is 40 ⁇ m or less, the excellent thermal conductivity of the graphite laminate can be exhibited when it is combined with the graphite laminate. Further, the thickness of the insulating layer is preferably 10 ⁇ m or more. When the thickness is 10 ⁇ m or more, sufficient adhesiveness can be maintained even when the graphite composite film is used in combination with a heat-generating component or a heat-dissipating component, and long-term reliability is excellent.
- These insulating layers may be directly formed on the graphite laminate by coating, printing, dipping, vapor deposition, or the like, or may be formed via an adhesive or adhesive.
- ⁇ Conductive layer> examples of the material for the conductive layer include copper and aluminum. These materials have excellent heat resistance, and sufficient long-term reliability even when a graphite composite film is used in combination with a heat-generating component or a heat-dissipating component. Is obtained.
- the thickness of the conductive layer is 40 ⁇ m or less, preferably 30 ⁇ m or less, more preferably 20 ⁇ m or less.
- the thickness is 40 ⁇ m or less, the excellent thermal conductivity of the graphite laminate can be exhibited when it is combined with the graphite laminate.
- the thickness of a conductive layer is good in it being 10 micrometers or more. When the thickness is 10 ⁇ m or more, sufficient adhesiveness can be maintained even when the graphite composite film is used in combination with a heat-generating component or a heat-dissipating component, and the long-term reliability is excellent.
- These conductive layers may be directly formed on the graphite laminate by coating, plating, sputtering, vapor deposition, or the like, or may be formed via an adhesive material or an adhesive material.
- the material for the adhesive layer include acrylic adhesives, silicone adhesives, etc. These materials have excellent heat resistance, and even when a graphite composite film is used in combination with heat-generating parts or heat-dissipating parts. Sufficient long-term reliability can be obtained. Moreover, the graphite composite film once attached may need to be removed in the case of an incorrect attachment position or repair after use. Acrylic adhesives and silicone adhesives are excellent in reusability and removability because they are excellent in repeated use and long-term reliability.
- the thickness of the adhesive layer is 40 ⁇ m or less, preferably 30 ⁇ m or less, and more preferably 20 ⁇ m or less. When the thickness is 40 ⁇ m or less, the excellent thermal conductivity of the graphite laminate can be exhibited when it is combined with the graphite laminate.
- the thickness of the adhesive layer is preferably 10 ⁇ m or more. When the thickness is 10 ⁇ m or more, sufficient adhesiveness can be maintained even when the graphite composite film is used in combination with a heat-generating component or a heat-dissipating component, and the long-term reliability is excellent.
- the adhesive layer is preferably a material including a base material.
- the stiffness of the graphite composite film is increased, and the peeling of the graphite laminate can be suppressed when the release liner is peeled off or when the graphite composite film once attached is peeled off again.
- each film constituting the graphite laminate may be easily peeled in layers, but the presence of the base material makes the peelability easy. It becomes possible to improve.
- the presence of the base material increases the strength of the graphite composite film, and it is possible to prevent the graphite laminate from being damaged at the time of attachment, mechanically crimped and fixed, or at the time of rework.
- the base material of the adhesive layer is preferably a material containing polyimide or polyethylene terephthalate.
- Polyimide and polyethylene terephthalate are excellent in heat resistance, strength, and dimensional stability. When combined with a graphite laminate, it does not degrade the thermal conductivity of the graphite laminate and prevents peeling. A graphite composite film having excellent properties can be realized.
- the thickness of the base material is preferably 6 ⁇ m or less.
- the thickness of the substrate is thin, it can be combined with the graphite composite without impairing the excellent thermal diffusibility of the graphite laminate.
- the thickness of the base material is increased, a force is easily applied to the base material of the pressure-sensitive adhesive layer when the release liner is peeled off or used in bending.
- the base material is strong in elongation, it is possible to follow the bending.
- the graphite laminate is vulnerable to bending, if the bending is performed to the same extent as the base material, the graphite laminate is likely to be wrinkled. Therefore, when applying a force to the graphite laminate rather than the base material of the adhesive layer, that is, by thinning the base material of the adhesive layer, when peeling the release liner or bending it, It is preferable to suppress wrinkles from entering the laminate.
- the insulating layer may be formed directly on the graphite film by coating, printing, dipping, or vapor deposition, or may be formed by transfer using a laminate.
- the graphite laminate, the heat transport structure, and the rod-shaped heat transport body of the present invention may have a bent shape. Having such a shape means that when the graphite laminate, the heat transport structure and the rod-shaped heat transport body of the present invention are mounted on various devices (for example, electronic devices or electrical devices), This is advantageous from the viewpoint of realizing downsizing and efficient heat dissipation of the device. This point will be described with reference to FIG.
- 28 (a) and 28 (b) are diagrams showing an example of the arrangement of the graphite laminate having bent portions in various devices, and are side views of the device including the graphite laminate.
- FIG. 28A two electronic components 550 are arranged inside the device, a high-temperature part 540 is arranged above one electronic component 550, and a low-temperature part is located below the other electronic component 550. 541 is arranged.
- the graphite laminate 501 has a stepped shape, the graphite laminate 501, the high temperature portion 540, the low temperature portion 541, and the electronic component 550 can be arranged in a narrow space, and the graphite laminate
- the high temperature part 540 and the low temperature part 541 can be reliably connected via the line 501.
- the graphite laminate 501 and the high temperature part 540 are arranged so as to be in close contact with each other. Furthermore, it is preferable that the graphite laminated body 501 and the low temperature part 541 are arrange
- the graphite laminate 501 and the electronic component 550 may be disposed so as to be in close contact with each other, or may be disposed at a desired distance. From the viewpoint of preventing heat from being transferred from the graphite laminate 501 to the electronic component 550, the graphite laminate 501 and the electronic component 550 are preferably arranged at a desired distance.
- one electronic component 550 is arranged inside the device, a high temperature part 540 is arranged beside one side surface of the electronic component 550, and beside the other side surface of the electronic component 550, A low temperature portion 541 is arranged.
- the graphite laminate 501 has a concave shape, the graphite laminate 501, the high temperature portion 540, the low temperature portion 541 and the electronic component 550 can be arranged in a narrow space, and the graphite laminate 501.
- the high-temperature part 540 and the low-temperature part 541 can be reliably connected via the.
- the graphite laminate 501 and the high temperature part 540 are arranged so as to be in close contact with each other. Furthermore, it is preferable that the graphite laminated body 501 and the low temperature part 541 are arrange
- the graphite laminate 501 and the electronic component 550 may be disposed so as to be in close contact with each other, or may be disposed at a desired distance. From the viewpoint of preventing heat from being transferred from the graphite laminate 501 to the electronic component 550, the graphite laminate 501 and the electronic component 550 are preferably arranged at a desired distance.
- thermocouple 325 was attached where the end 327 and the rod-shaped heat transporter 301 were in contact, and a thermocouple 326 was attached where the running water 323 and the end 328 were in contact.
- the temperature measured by the thermocouple 325 is the temperature T of the high temperature region, and the temperature measured by the thermocouple 326 is the temperature of the low temperature region (20 ° C.).
- the heat insulating material 324 was covered except for the low temperature portion of the rod-shaped heat transporter 301.
- the output Q of the heater 322 was adjusted so that the high-temperature part became a constant temperature.
- the output Q of the heater 322 adjusted so that the high temperature part becomes 100 ° C.
- the deformation rate was calculated by the following method. As shown in FIG. 26 (1), both ends of the rod-shaped heat transport body 301 are held by the first clamp 312 and the second clamp 313 so that the rod-shaped heat transport body 301 is parallel to the ground. After that, as shown in FIG. 26 (2), the second clamp 313 was removed. A vertical distance x between the position of the center of the end of the rod-shaped heat transporter before removing the holding and the position of the center of the end of the rod-shaped heat transporting body that hangs down after removing the holding; and The length L of the rod-shaped heat transporter was measured. And x / L was taken as the deformation rate of the rod-shaped heat transporter.
- the length of the portion of the rod-shaped heat transporter that is not held by the first clamp 312 and the second clamp 313 is the length L of the rod-shaped transporter. Stipulated. In other words, the total length of the rod-shaped heat transporter minus the length of the portion of the rod-shaped heat transporter held by the first clamp 312 and the second clamp 313 is the rod-shaped heat transporter. The length L of the transporter was defined.
- a graphite sheet (referred to as GS1) obtained by heat-treating a polymer film (polyimide film) having a thickness of 40 ⁇ m, a plane direction thermal conductivity of 1450 W / mK, a density of 2.1 g / cm 3 , and an electric conductivity of 14000 S / cm It was used.
- Example 1A 20 sheets of graphite sheets GS1 and PET films (thickness 5 ⁇ m, dielectric constant 3.2, melting point 260 ° C.) having a size of 200 mm ⁇ 200 mm are laminated alternately, and the laminate is heated to 250 ° C. Using a machine, a pressure of 0.5 MPa was applied for 1 minute to obtain a laminate (thickness 0.8 mm). The laminate was cut to produce a 2.7 ⁇ 0.8 ⁇ 90 mm rod-shaped heat transporter.
- the deformation rate was 1% or less.
- Example 2A 68 sheets of graphite sheets GS1 and PET films (thickness 5 ⁇ m, dielectric constant 3.2, melting point 260 ° C.) having a size of 200 mm ⁇ 200 mm were alternately laminated, and the laminate was heated to 250 ° C. Using a machine, a pressure of 0.5 MPa was applied for 1 minute to obtain a laminate (thickness 2.7 mm). The laminate was cut to produce a 2.7 ⁇ 0.8 ⁇ 90 mm rod-shaped heat transporter.
- the deformation rate was 1% or less.
- Example 3A 68 sheets of graphite sheets GS1 and PET films (thickness 5 ⁇ m, dielectric constant 3.2, melting point 260 ° C.) having a size of 200 mm ⁇ 200 mm were alternately laminated, and the laminate was heated to 250 ° C. Using a machine, a pressure of 0.5 MPa was applied for 1 minute to obtain a laminate (thickness 2.7 mm). This laminate was cut to produce a 2.7 ⁇ 2.7 ⁇ 90 mm rod-shaped heat transporter.
- the deformation rate was 1% or less.
- Example 4A The rod-shaped heat transporter obtained in Example 3A is polished, and the cross-section of the heat transporter is processed into a circular shape with a diameter of 2 mm (both the minor axis and the major axis are 2 mm), thereby producing the rod-shaped heat transporter. Produced.
- the deformation rate was 1% or less.
- Example 5A 20 sheets of graphite sheets GS1 and PET films (thickness 5 ⁇ m, dielectric constant 3.2, melting point 260 ° C.) having a size of 200 mm ⁇ 200 mm are laminated alternately, and the laminate is heated to 250 ° C. Using a machine, a pressure of 0.5 MPa was applied for 1 minute to obtain a laminate (thickness 0.8 mm). This laminate was cut to produce a 2.7 ⁇ 0.8 ⁇ 180 mm rod-shaped heat transporter.
- the deformation rate was 1% or less.
- the deformation rate was 1% or less.
- the deformation rate was 1% or less.
- Example B ⁇ B-1.
- Graphite sheet> (Basic structure of graphite sheet) The structure of the graphite sheet used in the examples is shown in Table 1 and below.
- Graphite sheet thickness Using a thickness gauge (HEIDENH: AIN-CERTO, manufactured by HEIDENHAIN Co., Ltd.), a sample of a graphite sheet cut into a shape of 50 mm ⁇ 50 mm has a thickness at any 10 points in a constant temperature room at 25 ° C. Was measured, and the thickness of the graphite sheet was calculated as an average value of the measured values.
- HEIDENH AIN-CERTO
- Graphite sheet density As for the density of the graphite sheet, the weight and thickness of a graphite sheet sample cut into a shape of 100 mm ⁇ 100 mm were measured, and the measured weight value was calculated as the calculated volume value (100 mm ⁇ 100 mm ⁇ thickness). ) To calculate.
- the electric conductivity of the graphite sheet was measured by applying a constant current by a four-probe method (for example, Loresta GP manufactured by Mitsubishi Chemical Analytech Co., Ltd.).
- the thermal conductivity in the plane direction of the graphite sheet was calculated by the following equation (1).
- A ⁇ ⁇ d ⁇ Cp (1)
- A the thermal conductivity of the graphite sheet
- ⁇ the thermal diffusivity of the graphite sheet
- d the density of the graphite sheet
- Cp the specific heat capacity of the graphite sheet.
- the thermal diffusivity of the graphite sheet is measured using a thermal diffusivity measuring device based on the optical alternating current method (for example, “LaserPit” manufactured by ULVAC-RIKO Co., Ltd.) for a graphite sheet sample cut into a 4 mm ⁇ 40 mm shape.
- the measurement was performed under an alternating current condition of 10 Hz in an atmosphere of 20 ° C.
- the weight and thickness of a graphite sheet sample cut into a shape of 100 mm ⁇ 100 mm were measured, and the measured weight value was calculated as the calculated volume value (100 mm ⁇ 100 mm ⁇ thickness). ) To calculate.
- the specific heat capacity of the graphite sheet was measured from 20 ° C. to 260 ° C. under a temperature rising condition of 10 ° C./min using a differential scanning calorimeter DSC220CU which is a thermal analysis system manufactured by SII Nano Technology.
- Adhesive layer> (Basic structure of adhesive layer) The composition of the adhesive layer used in the examples is shown in Table 2 and below.
- polyester adhesive polyethylene terephthalate, melting point 260 °
- PE polyethylene
- acrylic double-sided tape polyimide precursor
- rubber sheet silicone was used as the adhesive layer. Details of the physical properties of each adhesive layer are shown in Table 2. Moreover, the measuring method of each physical property is demonstrated below.
- Glass transition point of adhesive layer The glass transition point of the adhesive layer was measured by differential scanning calorimetry (DSC-50 manufactured by Shimadzu Corporation, temperature rising rate 1 ° C./min).
- Adhesive layer thickness Using a thickness gauge (HEIDENH: AIN-CERTO, manufactured by HEIDENHAIN Co., Ltd.), the thickness of the adhesive layer sample cut into a 50 mm ⁇ 50 mm shape at any 10 points in a constant temperature room at 25 ° C. was measured, and the thickness of the adhesive layer was calculated as an average value of the measured values.
- HEIDENH AIN-CERTO, manufactured by HEIDENHAIN Co., Ltd.
- the dielectric constant of the adhesive layer was measured at a frequency of 1 kHz using AS-4245 manufactured by Ando Electric Co., Ltd. after being allowed to stand for 24 hours at a temperature of 20 ° C. and a humidity of 60%.
- the water absorption rate of the adhesive layer was measured according to JIS K 7209 by comparing the mass of the adhesive layer in a dry state with the mass of the adhesive layer after being immersed in water for 24 hours.
- the adhesive strength of the adhesive layer was determined according to Method 1 “Testing method for peeling strength against test plate by 180 degrees” described in JIS-Z0237.
- a SUS plate described in JIS-Z0237 having a width of 50 mm, a length of 125 mm, a thickness of 1.1 mm, and a surface roughness Ra of 50 nm was washed with methanol.
- a protective layer of 20 mm ⁇ 300 mm was applied by two reciprocating pressures so that air could not enter the washed SUS plate with a 2 kg roller under conditions of an environmental temperature of 23 ° C. and a humidity of 50%.
- the obtained graphite sheets with an adhesive layer were laminated in the number shown in Table 3, and a pressure of 0.5 MPa was applied to the laminated body using a press machine for 1 minute, thereby biaxially.
- a graphite block in which graphite crystals were oriented was obtained.
- the obtained graphite block was cut with a tip saw at an angle of 90 ° with respect to the crystal plane of graphite to obtain a graphite laminate shown in Table 3.
- the crystal plane observed by an X-ray diffractometer manufactured by Rigaku Corporation was used as the crystal plane of graphite.
- the obtained graphite block was cut with a tip saw at an angle of 90 ° with respect to the crystal plane of graphite to obtain a graphite laminate shown in Table 3.
- the obtained graphite sheets with an adhesive layer were laminated in the number shown in Table 3, and a pressure of 100 ° C. and 0.5 MPa was applied to the laminate using a hot press machine for 10 minutes.
- a graphite block having graphite crystals oriented in the biaxial direction was obtained.
- the obtained graphite block was cut at an angle of 90 ° with respect to the crystal plane of graphite to obtain a graphite laminate shown in Table 3.
- the obtained graphite block was cut at an angle of 90 ° with respect to the crystal plane of graphite to obtain a graphite laminate shown in Table 3.
- a silicone adhesive was applied to both sides of the graphite sheet to a thickness of about 0.5 mm, and 17 graphite sheets and 18 rubber sheets were alternately stacked.
- the laminate was pressed from above and below (substantially perpendicular to the sheet surface of the graphite sheet) to bond the sheets together to obtain a laminate having a thickness of about 10 mm (the graphite sheet in the laminate is graphite).
- the ab plane of the crystal and the sheet plane of the graphite sheet are substantially parallel). This laminate was cut to obtain a graphite laminate having a thickness of 1 mm.
- Example 2 (Method for producing the graphite laminate of Example 18B)
- the laminated body after hot pressing was cut into the shape of FIG. 17 with an NC cutter, and 90 mm (long side direction of the surface perpendicular to the laminating direction) ⁇ 2.75 mm (surface perpendicular to the laminating direction) Of graphite) having a bent portion of 0.8 mm (stacking direction).
- Example 2 (Method for producing the graphite laminate of Example 19B)
- Example 2 After hot pressing using a bending mold as shown in FIG. 6 at the time of hot pressing, it was cut perpendicularly to the stacking direction with a single wire saw, and 90 mm (stacking direction) as shown in FIG.
- the graphite laminated body which has a bending part of the long side direction of a surface perpendicular
- the thickness of the graphite sheet, which is the material of the graphite laminate, is A1 [ ⁇ m], and the number of layers is B1 [sheets].
- the thickness of the adhesive layer, which is the material of the graphite laminate, is A2 [ ⁇ m]
- the number of layers is B2 [sheets].
- the thermal conductivity in the plane direction of the graphite laminate can be calculated by the following equation (2).
- a 1 ⁇ 1 ⁇ d 1 ⁇ Cp 1 (2)
- a 1 is the thermal conductivity of the graphite laminate
- ⁇ 1 is the thermal diffusivity of the graphite laminate
- d 1 is the density of the graphite laminate
- Cp 1 is the specific heat capacity of the graphite laminate.
- the thermal diffusivity, density, and specific heat capacity of a graphite laminated body can be calculated
- the thermal diffusivity of the graphite laminate was measured using a thermal diffusivity measuring device based on the optical alternating current method (for example, “LaserPit” manufactured by ULVAC-RIKO Co., Ltd.) for a graphite sheet sample cut into a 4 mm ⁇ 40 mm shape. It can be measured under an AC condition of 10 Hz in an atmosphere of 20 ° C.
- the optical alternating current method for example, “LaserPit” manufactured by ULVAC-RIKO Co., Ltd.
- the density of the graphite laminate was determined by measuring the weight and thickness of a sample of the graphite laminate cut into a shape of 100 mm ⁇ 100 mm, and using the measured weight value as the calculated volume value (100 mm ⁇ 100 mm ⁇ It can be calculated by dividing by (thickness).
- the specific heat capacity of the graphite laminate can be measured from 20 ° C. to 260 ° C. under a temperature rising condition of 10 ° C./min using a differential scanning calorimeter DSC220CU which is a thermal analysis system manufactured by SII Nano Technology Co., Ltd. .
- Thermal conductivity of graphite laminate (theoretical value)
- the thermal conductivity (theoretical value) of the graphite laminate was calculated by “thermal conductivity of graphite sheet ⁇ total thickness of graphite sheet ⁇ thickness of laminate”.
- thermal conductivity of graphite laminate (close to the theoretical value)
- the thermal conductivity (closeness to the theoretical value) of the graphite laminate was calculated by “actual measured value of thermal conductivity ⁇ thermal conductivity (theoretical value)”.
- the case where wrinkles enter the entire adhesive layer is determined as “D”, and when the graphite sheet and the adhesive layer are laminated, wrinkles enter a part of the adhesive layer. It is determined as “C”, and when the graphite sheet and the adhesive layer are laminated, it is determined as “B” when it is difficult to enter the adhesive layer, and when the graphite sheet and the adhesive layer are laminated, the adhesive layer has The case where it did not enter was determined as “A”.
- the case where the graphite sheet layer is peeled is determined as “F”, and the case where the graphite sheet layer is partially peeled is determined as “E”.
- the case where the laminate is deformed is determined as “D”, and the graphite sheet is not peeled, but the case where the graphite laminate is slightly deformed is determined as “C”, the graphite sheet is not peeled, and the graphite laminate is The case where it was not deformed was determined as “B”.
- the case where the graphite sheet was not peeled off and the graphite laminate was not deformed was determined as “A”.
- the sample whose surface shape is a square of 16 mm (short direction) ⁇ 65 mm (longitudinal direction), the end portion 10 mm in the longitudinal direction is fixed with tape, and the sample is 4 cm away from the fixed end portion.
- a circular weight having a diameter of 20 mm was placed on the surface. The weight and the sample were fixed to each other with a tape so that the weight did not slide off the sample. Further, the weight and the sample were arranged so that the center of the weight and the center of the sample overlapped.
- the weight of the weight is W (g)
- the thickness of the sample is T (mm)
- the width of the sample is L (mm)
- the width L (mm) of the sample is the short direction of the sample.
- the length is 16 (mm)
- the thickness T (mm) of the sample is “thickness (mm)” shown in Table 3.
- the value of “thickness (mm)” shown in Table 3 may be substituted for “L” in the above formula.
- Examples 1B to 4B and 9B to 19B a displacement of 12 mm was observed.
- Examples 5B and 6B a displacement of 14 mm was observed.
- Examples 7B and 8B a displacement of 10 mm was observed.
- Comparative Examples 1B to 6B a displacement of 22 mm was observed.
- Comparative Example 7B a displacement of 18 mm was observed.
- the displacement value is smaller in the example than in the comparative example, and this indicates that the graphite laminate is harder in the example than in the comparative example. It can be said that the harder the graphite laminate, the easier the handling of the graphite laminate and the better.
- thermal conductivity (close to the theoretical value) close to “1.00” indicates that the thermal conductivity of the graphite laminate is high.
- Graphite sheet> (Basic structure of graphite sheet)
- the graphite sheet used in the examples was a graphite sheet obtained by heat-treating a polymer film (polyimide film) and having a thickness of 40 ⁇ m, a width of 210 mm, a length of 260 mm, and a plane direction thermal conductivity of 1300 W / mK.
- Graphite sheet thickness Using a thickness gauge (HEIDENH: AIN-CERTO, manufactured by HEIDENHAIN Co., Ltd.), the thickness of a graphite sheet sample cut into a 50 mm ⁇ 50 mm shape was measured at any 10 points in a constant temperature room at 25 ° C. And the thickness of the graphite sheet was computed as an average value of the said measured value.
- HEIDENH AIN-CERTO, manufactured by HEIDENHAIN Co., Ltd.
- Adhesive layer> (Basic structure of adhesive layer)
- the adhesive layer material used in the examples was PET (polyethylene terephthalate, melting point 260 ° C.). Moreover, the measuring method of each physical property is demonstrated below.
- the melting temperature of the adhesive layer was measured with a differential scanning calorimeter (DSC-50 manufactured by Shimadzu Corporation) in accordance with JIS K7121.
- Graphite laminate> Metals for producing graphite laminates of Examples 1C to 11C and Reference Examples 1C to 11C
- Graphite sheets and adhesive layer materials were alternately laminated in the number shown in Table 4 to produce a laminate.
- a predetermined temperature shown in Table 4 a predetermined pressure was applied to the laminate for a predetermined time to obtain a graphite laminate in which graphite crystals were oriented in biaxial directions.
- 2nd pressurization 2nd pressurization was performed after the 1st pressurization.
- the first pressure was continuously applied to the laminate during the temperature range of “20 ° C. to less than 250 ° C.”
- the second pressure was continuously applied to the laminate.
- PET polyethylene terephthalate, melting point 260 ° C.
- [(melting temperature of adhesive layer material) ⁇ 20 ° C.] is 240 ° C.
- the pressurization at “240 ° C. to less than 250 ° C.” included in “first pressurization (° C.)” in Tables 4 and 5 is applied in addition to the first pressurization and the second pressurization. It can be considered as a pressure (for example, a third pressure).
- Examples 12C to 23C and Reference Examples 12C to 22C in which the laminates are laminated in multiple stages the graphite laminates corresponding to the laminates in which the lamination positions in one batch are at the upper, middle, and lower portions are respectively extracted, and the graphite The SEM image of the laminate was observed to determine the adhesion of the graphite laminate.
- the upper part refers to the laminate at the first stage from the top
- the middle part refers to the position near the center
- the lower part refers to the laminate at the first stage from the bottom.
- Example 1C when Example 1C is compared with Reference Example 1C, in Example 1C, the step of extracting air from the laminated body by the first pressurization is performed, and the second pressurization is performed at a pressure higher than the first pressurization.
- the thermal conductivity in the thickness direction within the graphite laminate was improved, and the heat transfer of the graphite laminate was excellent.
- Example 2C is compared with Reference Example 1C
- Example 3C is more effective.
- Example 4C was compared with Reference Example 1C
- Example 4C was better.
- Example 5C was compared with Reference Example 1C
- Example 5C was better than Example 6C and Reference Example 1C.
- Example 6C is better.
- Example 7C is better.
- Example 8C is better.
- Example 9C was compared with Reference Example 1C
- Example 9C was better.
- Example 10C was compared with Reference Example 1C
- Example 10C was better than Example 11C.
- Example 11C compares Example 12C with Reference Example 12C.
- Write Example 12C if the is, the better the thickness direction of the thermally conductive graphite laminate was excellent in terms of heat transmitted ease.
- the present invention can be used for heat transport materials such as electronic devices. Further, the present invention can be suitably used as a thermal highway used for a smartphone, a tablet, a fanless notebook computer, etc., in which the heat generation amount of the CPU is larger.
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Abstract
Description
λa/λb>0.7 式(1)
式(1)において、λaは、上記高温部位の温度が100℃であるときの熱伝導率を表し、λbは上記高温部位の温度が50℃であるときの熱伝導率を表す。
上記グラファイト積層体は、当該グラファイト積層体の少なくとも2つ以上の屈曲部において折れ曲げられた形状を有しており、
上記屈曲部の各々は、以下の(a)~(c)の何れかであることを特徴としている:
(a)上記グラファイト積層体を、上記X軸の方向または上記Y軸の方向に向かって屈曲させた第1の屈曲部、
(b)上記グラファイト積層体を、上記Z軸の方向に向かって屈曲させた第2の屈曲部、
(c)上記グラファイト積層体を、上記X軸の方向または上記Y軸の方向に向かって屈曲させ、かつ、上記Z軸の方向に向かって屈曲させた第3の屈曲部。
上記グラファイト積層体は、当該グラファイト積層体の少なくとも1つ以上の屈曲部において折れ曲げられた形状を有しており、
上記屈曲部の各々は、以下の(c)であることを特徴としている:
(c)上記グラファイト積層体を、上記X軸の方向または上記Y軸の方向に向かって屈曲させ、かつ、上記Z軸の方向に向かって屈曲させた第3の屈曲部。
上記屈曲部形成工程は、2つ以上の屈曲部を有するグラファイト積層体を形成する、以下の(d)~(h)の屈曲部形成工程の少なくとも1つを包含することが好ましい:
(d)加熱および加圧された上記積層物を上記Z軸の方向に切断して、上記積層物から上記グラファイト積層体を切り出すことにより、上記グラファイト積層体に、上記X軸の方向または上記Y軸の方向に向かって屈曲した第1の屈曲部を形成する、第1の屈曲部形成工程、
(e)屈曲した形状を有する加圧治具によって、加熱および加圧された上記積層物を加圧することにより、上記グラファイト積層体に、上記Z軸の方向に向かって屈曲した第2の屈曲部を形成する、第2の屈曲部形成工程、
(f)屈曲した形状を有する加圧治具によって、加熱および加圧された上記積層物を加圧して、当該積層物をZ軸の方向に向かって屈曲させた後で、当該積層物を上記Z軸の方向に切断して、当該積層物から上記グラファイト積層体を切り出すことにより、上記グラファイト積層体に、上記Z軸の方向に向かって屈曲した第2の屈曲部を形成する、第3の屈曲部形成工程、
(g)加熱および加圧された上記積層物を上記Z軸の方向に切断して、上記積層物から、上記X軸の方向または上記Y軸の方向に向かって屈曲したグラファイト積層体の前駆体を切り出した後で、屈曲した形状を有する加圧治具によって、当該グラファイト積層体の前駆体を加圧することにより、上記グラファイト積層体に、上記X軸の方向または上記Y軸の方向に向かって屈曲し、かつ、上記Z軸の方向に向かって屈曲した第3の屈曲部を形成する、第4の屈曲部形成工程、
(h)屈曲した形状を有する加圧治具によって、加熱および加圧された上記積層物を加圧して、当該積層物をZ軸の方向に向かって屈曲させた後で、当該積層物を上記Z軸の方向に対して斜めに切断して、当該積層物から上記グラファイト積層体を切り出すことにより、上記グラファイト積層体に、上記X軸の方向または上記Y軸の方向に向かって屈曲し、かつ、上記Z軸の方向に向かって屈曲した第3の屈曲部を形成する、第5の屈曲部形成工程。
上記屈曲部形成工程は、1つ以上の屈曲部を有するグラファイト積層体を形成する、以下の(g)および(h)の屈曲部形成工程の少なくとも1つを包含することが好ましい:
(g)加熱および加圧された上記積層物を上記Z軸の方向に切断して、上記積層物から、上記X軸の方向または上記Y軸の方向に向かって屈曲したグラファイト積層体の前駆体を切り出した後で、屈曲した形状を有する加圧治具によって、当該グラファイト積層体の前駆体を加圧することにより、上記グラファイト積層体に、上記X軸の方向または上記Y軸の方向に向かって屈曲し、かつ、上記Z軸の方向に向かって屈曲した第3の屈曲部を形成する、第4の屈曲部形成工程、
(h)屈曲した形状を有する加圧治具によって、加熱および加圧された上記積層物を加圧して、当該積層物をZ軸の方向に向かって屈曲させた後で、当該積層物を上記Z軸の方向に対して斜めに切断して、当該積層物から上記グラファイト積層体を切り出すことにより、上記グラファイト積層体に、上記X軸の方向または上記Y軸の方向に向かって屈曲し、かつ、上記Z軸の方向に向かって屈曲した第3の屈曲部を形成する、第5の屈曲部形成工程。
本発明は、ロッド状の熱輸送体であって、該ロッド状の熱輸送体は、熱輸送体の一方の端部を高温部位に接触させ、かつ他方の端部を20℃に保たれた低温部位に接触させて測定される熱伝導率において、式(1)の関係を満足するロッド状の熱輸送体である。
λa/λb>0.7 式(1)
式(1)において、λaは高温部位の温度が100℃であるときの熱伝導率、λbは高温部位の温度が50℃であるときの熱伝導率を表す。
式(1)において、λaは前記高温部位の温度が100℃であるときの熱伝導率を表し、λbは前記高温部位の温度が50℃であるときの熱伝導率を表す。
1)ロッド状の熱輸送体301の端部328を流水323(低温部位)と接触させて、端部328の温度を20℃に保つ。
2)ロッド状の熱輸送体301の端部327にヒーター322(高温部位)を取り付ける(換言すれば、端部327をヒーター322(高温部位)と接触させる)。熱電対325を、端部327とロッド状の熱輸送体301とが接するところに取り付け、熱電対326を、流水323と端部328とが接するところに取り付ける。熱電対325で測定される温度が高温部位の温度Tであり、熱電対326で測定される温度が、低温部位の温度(20℃)である。
3)ロッド状の熱輸送体301の低温部分以外を断熱材324で覆う。
4)高温部位が一定温度となるように、ヒーター322の出力Qを調整する。
このとき、熱伝導率λは、断面Sと軸方向の長さLとを用いて、
λ=Q×L/[S(T-20℃)]
と算出することができる。
a)グラファイトシートを粉砕し、金型に充填した後、プレス加工する方法、
b)グラファイトシートと、必要に応じて接着層とを任意形状に折り曲げながら、箱形に押し込んだ後、プレスする方法、
c)グラファイトシートと接着層とを交互に積層し、加熱および/または加圧などを行い、グラファイトシートと接着層とを接着させ、当該積層体をロッド状になるように切断する方法、などが挙げられるが、これに限定されない。この中でも、ロッドの大きさや形状を自由に設計でき、かつ熱伝導率に優れたロッド状の熱輸送体を容易に得ることができるという点から、c)の方法が好ましい。c)の方法により、層状構造となったロッド状熱輸送体を得ることができる。
〔B-1.グラファイト積層体〕
本実施の形態のグラファイト積層体は、交互に積層されているグラファイトシートと接着層とを含むグラファイト積層体(または、グラファイトシートと接着層とが交互に積層されてなるグラファイト積層体)である。上記接着層は、熱可塑性樹脂および熱硬化性樹脂のうちの少なくとも1つの樹脂を含むものであってもよい。更に、上記接着層は、吸水率が2%以下のものであり、かつ、厚さが15μm未満のものであってもよい。上記グラファイト積層体に含まれる上記グラファイトシートの積層数は、3層以上であり得る。当該グラファイト積層体は、更に、上記グラファイトシートと上記接着層とが交互に積層された積層物を圧縮して得られるものであってもよい。なお、上述した接着層の厚さは、完成品であるグラファイト積層体の中に組み込まれている状態の接着層の厚さを意図し、完成品であるグラファイト積層体の中に組み込まれる前の接着層の厚さを意図するものではない。但し、完成品であるグラファイト積層体の中に組み込まれている状態の接着層の厚さと、完成品であるグラファイト積層体の中に組み込まれる前の接着層の厚さとは、略同一である。
(グラファイト積層体の基本構造)
グラファイト積層体は、グラファイトシートと、接着層とが、交互に積層されてなるものである。なお、グラファイトシートと接着層との間には、他の構成が挟まれていてもよいし、他の構成が挟まれていなくてもよい。
グラファイト積層体の厚さ(換言すれば、図1のZ軸の方向の長さ)は、特に限定されないが、0.5mm以上であることが好ましく、0.6mm以上であることがより好ましく、0.7mm以上であることがより好ましく、0.8mm以上であることがより好ましい。グラファイト積層体の厚さが0.5mm以上であれば、輸送できる熱量が多くなり、発熱量が大きな電子機器にも適用することができる。グラファイト積層体の厚さの上限値は、特に限定されないが、電子機器の薄型化という観点からは、10mm以下であってもよいし、7.5mm以下であってもよいし、5mm以下であってもよいし、2.5mm以下であってもよいし、1mm以下であってもよい。
グラファイト積層体は、当該グラファイト積層体に設けられた少なくとも1つ(例えば、1つ以上、または、2つ以上)の屈曲部において折れ曲げられた形状を有し得る。つまり、本実施の形態のグラファイト積層体は、屈曲前のグラファイト積層体を屈曲部にて折り曲げたものであり得る。電子機器の内部では、熱源にて発生した熱を温度の低い部分に移動させることで、熱輸送が可能になる。しかしながら、温度の低い部分と熱源とを、直線的に接続できるとは限らない。そこで、グラファイト積層体に屈曲部を形成しておくことで、熱源にて発生した熱をより温度の低い部分に容易に移動させることができ、これによって、熱輸送能力を更に向上させることができる。つまり、熱源と、より温度の低い部分との配置関係の自由度を、上げることができる。
(a)上記グラファイト積層体を、上記X軸の方向または上記Y軸の方向に向かって屈曲させた第1の屈曲部、
(b)上記グラファイト積層体を、上記Z軸の方向に向かって屈曲させた第2の屈曲部、
(c)上記グラファイト積層体を、上記X軸の方向または上記Y軸の方向に向かって屈曲させ、かつ、上記Z軸の方向に向かって屈曲させた第3の屈曲部。
グラファイト積層体は、樹脂(例えば、PET(polyethylene terephthalate)、PE(polyethylene)またはPI(polyimide)など)、または、金属(例えば、銅、ニッケルまたは金など)で被覆されたものであることが好ましい。グラファイトシートは、層状化合物であるために、擦れなどによって粉落ちが発生しやすい。そして、グラファイトシートは電気伝導性を有するため、粉落ちが発生すると、電子機器のショートを発生させる。
グラファイト積層体の吸水率は、特に限定されないが、0.25%以下であることが好ましく、0.20%以下であることが更に好ましく、0.10%以下であることが最も好ましい。グラファイト積層体の吸水率が0.25%以下であれば、グラファイト積層体の製造時や、グラファイト積層体を熱輸送機構として使用している時に、グラファイト積層体内の水が気化して発生するガス(アウトガス)の量が少ないので、グラファイト積層体の内部に空隙が生じることを防ぐことができる。なお、グラファイト積層体の吸水率は、以下の式にて算出することができる。つまり、
(グラファイト積層体の吸水率)=(接着層の吸水率)×(接着層の厚さ)/[(接着層の厚さ)+(グラファイトシートの厚さ)] ・・・・・(式)。
グラファイト積層体は、グラファイト積層体が地面に対して水平になるように上記グラファイト積層体の一方の端部を固定した後、固定した上記端部から4cm離れた位置におけるグラファイト積層体の断面に対して、当該断面1mm2あたり0.7gの荷重をかけたときに、上記断面の変位が15mm以下、好ましくは14mm以下、より好ましくは13mm以下、より好ましくは12mm以下、より好ましくは11mm以下、より好ましくは10mm以下、より好ましくは9mm以下、より好ましくは8mm以下、より好ましくは7mm以下、より好ましくは6mm以下、より好ましくは5mm以下、より好ましくは4mm以下、より好ましくは3mm以下、より好ましくは2mm以下、最も好ましくは1mm以下のものである。グラファイト積層体が固いほど、換言すれば、グラファイト積層体の形状変化が少ないほど、グラファイト積層体の取り扱いが容易となり、好ましい。
(グラファイトシートの種類)
本発明におけるグラファイトシートは、特に限定されず、高分子系グラファイトシート、または、原料である天然黒鉛をエキスパンドして得られるグラファイトシート、等を用いることができる。高分子系グラファイトシートは、強度が高く、かつ、高い熱伝導性を有しているので、グラファイト積層体におけるより高い強度、および、より高い熱輸送能力を実現することができるため、好ましい。
本発明におけるグラファイトシートの製造方法は、特に限定されない。
本発明におけるグラファイトシートの面方向の熱伝導率は、1000W/(m・K)以上であることが好ましく、1100W/(m・K)以上であることがより好ましく、1200W/(m・K)以上であることがさらに好ましく、1300W/(m・K)以上であることがさらに好ましい。
本発明におけるグラファイトシートの厚さは、特に限定されないが、好ましくは10μm以上200μm以下であり、より好ましくは12μm以上150μm以下であり、より好ましくは15μm以上100μm以下であり、より好ましくは20μm以上80μm以下である。グラファイトシートの厚さが10μm以上であれば、グラファイト積層体に含まれるグラファイトシートの積層枚数を削減することができ、熱伝導率の低い接着層の積層枚数を減らすことができる。また、グラファイトシートの厚さが、200μm以下であれば、グラファイト積層体の高い熱伝導率を実現することができる。
本発明におけるグラファイトシートの電気伝導率は、特に限定されないが、1000~25000S/cmが好ましく、2000~20000S/cmがより好ましく、5000~18000S/cmがより好ましく、10000~17000S/cmがより好ましい。グラファイトシートの電気伝導率が1000~25000S/cmであれば、グラファイトシートと接着層との間で、適度な密着性と適度な滑り性とを確保でき、接着層とグラファイトシートとの重ね合わせ(特に、薄い接着層との重ね合わせ)に優れるので好ましい。
本発明におけるグラファイトシートの密度は、特に限定されないが、0.8g/cm3以上が好ましく、1.0g/cm3以上が好ましく、1.5g/cm3以上がより好ましく、2.0g/cm3以上がより好ましく、2.5g/cm3以上がより好ましい。グラファイトシートの密度が0.8g/cm3以上であれば、グラファイトシート自体の自己支持性に優れるので好ましい。
本発明におけるグラファイトシートの表面粗さは、特に限定されないが、5μm以下が好ましく、2.0μm未満がより好ましく、1.5μm以下がより好ましく、1.0μm未満がより好ましい。グラファイトシートの表面粗さが5μm以下であれば、グラファイトシートと接着層との間で、適度な密着性と適度な滑り性とを確保でき、接着層とグラファイトシートとの重ね合わせ(特に、薄い接着層との重ね合わせ)に優れるので好ましい。
グラファイトシートを10層以上といった多層に積層する場合や、100mm角以上といった大面積のグラファイトシートを積層する場合、加熱および加圧を伴う接着では、接着層からわずかに発生するガスや各層間に僅かに巻き込んだ空気が膨張し、部分的に膨れが発生してしまう場合がある。これは、グラファイトシートの高いガスバリア性によるものである。
(接着層の種類)
本発明における接着層は、熱硬化性樹脂、または、熱可塑性樹脂を用いることができる。なお、接着層の材料としては、フィルム状のものを用いることも可能であるし、ワニス状のものを用いることも可能である。
本発明における接着層の厚さは、15μm未満であり得る。具体的に、本発明における接着層の厚さは、0.1μm以上15μm未満が好ましく、1μm以上15μm未満がより好ましい。更に具体的に、本発明における接着層の厚さは、0.1μm以上10μm未満が好ましく、1μm以上10μm未満がより好ましく、1μ以上9μm以下がより好ましく、1μm以上7μm以下がより好ましい。接着層の厚さが15μm未満(より好ましくは、10μm未満)であれば、接着層の熱伝導率は、グラファイトシートの熱伝導率に比べて、はるかに小さくなる。そのため、接着層の厚さを15μm未満(より好ましくは、10μm未満)に制御することで、グラファイトシート同士の間の伝熱を阻害することなく良好に熱を伝達することができる。接着層の厚さが1μm以上であれば、接着層によってグラファイトシート表面の凹凸を吸収し、グラファイトシートと接着層との間の接触熱抵抗を低減することができ、効率的に熱を伝達することができる。また、接着層が1μm以上あれば、接着層が良好な接着性を示すことができる。また、上述した接着層の厚さであれば、グラファイト積層体の熱伝導率を、理論値に近い値にすることができる。
本発明における接着層の吸水率は、2%以下であり得る。更に具体的に、本発明における接着層の吸水率は、1.5%以下がより好ましく、1.0%以下がより好ましく、0.4%以下がより好ましく、0.1%以下がより好ましい。接着層の吸水率が2%以下であれば、グラファイト積層体の製造時や、グラファイト積層体を熱輸送機構として使用している時に、接着層に含まれる水が気化してガス(アウトガス)が発生する量が少ないので、グラファイト積層体の内部に空隙が生じることを防ぐことができる。
本発明における接着層の誘電率は、特に限定されないが、1.0~5.0が好ましく、2.0~4.0がより好ましく、2.5~3.6がより好ましい。接着層の誘電率が1.0~5.0であれば、静電気によって接着層が反発し、離れ易くなるので好ましい。
接着層は、加熱によって接着性を発現し、接着工程において、接着性を有しているものが好ましい。よって、接着層としては、粘着剤、接着剤、または、高分子フィルムなどを用いることができるが、25℃での接着力が1N/25mm以下のものが好ましく、25℃での接着力が0.5N/25mm以下のものがより好ましく、更に具体的に、接着層は、25℃での接着力が1N/25mm以下のもの、または、25℃での接着力が0.5N/25mm以下のものであり、かつ、加熱により接着性を発現するものが好ましい。
本発明における接着層の破断強度は、特に限定されないが、0.1~10GPaが好ましく、0.2~5.0GPaがより好ましく、0.2~4.7GPaがより好ましく、1.0~4.7GPaがより好ましい。接着層の破断強度が0.1GPa以上であれば、フィルムの積層時に破れ難いので好ましい。
(グラファイト積層体の製造方法の基本構成)
グラファイト積層体の積層方向の厚さが厚くなると(例えば、0.5mm以上)、グラファイト積層体の柔軟性が低下し、グラファイト積層体を形成した後で、当該グラファイト積層体を曲げることが難しくなる。
積層工程は、グラファイトシートと接着層とを交互に積層して積層物を形成する工程である。
接着工程は、積層工程にて形成された積層物を(i)加圧(換言すれば、圧縮)、好ましくは、(ii)加熱および加圧(換言すれば、圧縮)することによって、グラファイトシートと接着層とを接着させてグラファイト積層体を形成する工程である。
屈曲部は、グラファイト積層体を製造する過程で、グラファイト積層体の前駆体を折り曲げることによって形成されてもよいし、グラファイト積層体を製造した後、当該グラファイト積層体を折り曲げることによって形成されてもよい。例えば、グラファイトシートと接着層とを積層した後、当該積層物に対して加熱および加圧して、当該加圧によって、形成途中のグラファイト積層体(換言すれば、グラファイト積層体の前駆体)を折り曲げ、これによって屈曲部を形成してもよい。または、グラファイトシートと接着層とを積層した後、当該積層物に対して加熱および加圧してグラファイト積層体を形成する。形成されたグラファイト積層体に対して別途加圧して、形成されたグラファイト積層体を折り曲げ、これによって屈曲部を形成してもよい。
(d)加熱および加圧された上記積層物を上記Z軸の方向に切断して、上記積層物から上記グラファイト積層体を切り出すことにより、上記グラファイト積層体に、上記X軸の方向または上記Y軸の方向に向かって屈曲した第1の屈曲部を形成する、第1の屈曲部形成工程、
(e)屈曲した形状を有する加圧治具によって、加熱および加圧された上記積層物を加圧することにより、上記グラファイト積層体に、上記Z軸の方向に向かって屈曲した第2の屈曲部を形成する、第2の屈曲部形成工程、
(f)屈曲した形状を有する加圧治具によって、加熱および加圧された上記積層物を加圧して、当該積層物をZ軸の方向に向かって屈曲させた後で、当該積層物を上記Z軸の方向に切断して、当該積層物から上記グラファイト積層体を切り出すことにより、上記グラファイト積層体に、上記Z軸の方向に向かって屈曲した第2の屈曲部を形成する、第3の屈曲部形成工程、
(g)加熱および加圧された上記積層物を上記Z軸の方向に切断して、上記積層物から、上記X軸の方向または上記Y軸の方向に向かって屈曲したグラファイト積層体の前駆体を切り出した後で、屈曲した形状を有する加圧治具によって、当該グラファイト積層体の前駆体を加圧することにより、上記グラファイト積層体に、上記X軸の方向または上記Y軸の方向に向かって屈曲し、かつ、上記Z軸の方向に向かって屈曲した第3の屈曲部を形成する、第4の屈曲部形成工程、
(h)屈曲した形状を有する加圧治具によって、加熱および加圧された上記積層物を加圧して、当該積層物をZ軸の方向に向かって屈曲させた後で、当該積層物を上記Z軸の方向に対して斜めに切断して、当該積層物から上記グラファイト積層体を切り出すことにより、上記グラファイト積層体に、上記X軸の方向または上記Y軸の方向に向かって屈曲し、かつ、上記Z軸の方向に向かって屈曲した第3の屈曲部を形成する、第5の屈曲部形成工程。
(e’)2カ所が屈曲した形状を有する加圧治具(換言すれば、階段状に屈曲した形状を有する加圧治具)によって、加熱および加圧された上記積層物を加圧することにより、上記グラファイト積層体に、上記Z軸の方向に向かって屈曲した、2つの第2の屈曲部(換言すれば、逆方向に折れ曲がった、2つの第2の屈曲部)を形成する、第6の屈曲部形成工程。
(熱輸送用構造物の基本構成)
上述した本発明のグラファイト積層体は、主に電子機器の熱輸送用材料として用いることができる。
高温部位に対するグラファイト積層体の配置について説明する。
グラファイト積層体の積層面を高温部位に対向させる場合、グラファイト積層体の積層方向の長さが、グラファイト積層体の積層方向と垂直な面(当該面の形状は、例えば、長方形)の短辺の長さよりも長いことが好ましい。より具体的に、図15および16において、グラファイト積層体1のZ軸の方向の長さは、グラファイト積層体1のX軸方向の長さよりも厚いことが好ましい。積層方向の長さを、積層方向と垂直な面の短辺の長さよりも長くすることで、グラファイト積層体の受熱面から、当該受熱面の反対側の面への熱移動を良好にすることができ、これによって、低温部位への熱輸送をより効果的に行うことができる。
上記接着層は、熱可塑性樹脂および/または熱硬化性樹脂を含み、
上記接着層は、吸水率が2%以下であり、かつ、厚さが10μm未満であり、
上記グラファイトシートの積層数が、5層以上であることを特徴とする、グラファイト積層体。
上記接着層は、熱可塑性樹脂および/または熱硬化性樹脂を含み、
上記接着層は、吸水率が2%以下であり、
上記グラファイト積層体の厚さは、グラファイトシートの原料シートの厚さと、接着層の厚さとの合計よりも小さく、
上記グラファイトシートの積層数が、5層以上であることを特徴とする、グラファイト積層体。
上記未接着部は、上記グラファイト積層体の長手方向の両端部以外に形成されていることを特徴とする、<7>~<11>の何れかに記載のグラファイト積層体。
上記グラファイト積層体の一方の端部は、上記発熱素子が発する熱によって昇温する部位である高温部位に配置されており、
上記グラファイト積層体の他方の端部は、上記高温部位よりも温度が低い部位である低温部位に配置されていることを特徴とする、放熱構造物。
各層を、加熱と加圧とにより接着させる接着工程と、を有することを特徴とするグラファイト積層体の製造方法。
上記接着工程では、加熱と加圧とにより、各層を一括して接着させることを特徴とする、<19>に記載のグラファイト積層体の製造方法。
〔C-1.グラファイト積層体〕
本実施の形態のグラファイト積層体は、交互に積層されているグラファイトシートと接着層とを含むグラファイト積層体(または、グラファイトシートと接着層とが交互に積層されてなるグラファイト積層体)であって、接着層の材料である接着層材料、または、接着層は、熱可塑性樹脂および熱硬化性樹脂のうちの少なくとも1つの樹脂を含むものである。
(グラファイト積層体の基本構造)
グラファイト積層体は、グラファイトシートと、接着層とが、交互に積層されてなるものである。なお、グラファイトシートと接着層との間には、他の構成が挟まれていてもよいし、他の構成が挟まれていなくてもよい。
グラファイト積層体の厚み(換言すれば、図20のZ軸の方向の長さ)は、特に限定されず、0.1mm以上であることが好ましく、0.4mm以上であることがより好ましく、0.6mm以上であることがより好ましく、0.8mm以上であることがより好ましい。グラファイト積層体の厚みが0.1mm以上であれば、輸送できる熱量が多くなり、発熱量が大きな電子機器にも適用することができる。グラファイト積層体の厚みの上限値は、特に限定されず、電子機器の薄型化という観点からは、10mm以下であってもよいし、7.5mm以下であってもよいし、5mm以下であってもよいし、2.5mm以下であってもよいし、1mm以下であってもよい。
グラファイト積層体は、当該グラファイト積層体に設けられた少なくとも1つ(例えば、1つ以上、または、2つ以上)の屈曲部において折れ曲げられた形状を有していてもよい。つまり、グラファイト積層体は、屈曲前のグラファイト積層体を屈曲部にて折り曲げたものであり得る。電子機器の内部では、熱源にて発生した熱を温度の低い部分に移動させることで、温度上昇の防止が可能になる。しかしながら、温度の低い部分と熱源とを、直線的に接続できるとは限らない。そこで、グラファイト積層体に屈曲部を形成しておくことで、熱源にて発生した熱をより温度の低い部分に移動させることができ、これによって、熱輸送能力を更に向上させることができる。つまり、熱源と、より温度の低い部分との配置関係の自由度を、上げることができる。なお、屈曲部の具体的な構成としては、実施の形態Bにて説明した屈曲部の構成を採用することができる。
〔実施の形態C〕のグラファイト積層体の被覆に関しては、〔実施の形態B〕の(グラファイト積層体の被覆)の欄に記載の構成と同じ構成を採用することができる。
グラファイト複合品は、グラファイト積層体の少なくとも片面に、少なくとも粘着材または接着材を有するシートが貼り合わせられたものである。この粘着材または接着材を有するシートによって、コンピュータなどの各種電子・電気機器に搭載されている半導体素子や他の発熱部品などに、熱輸送のためのグラファイト積層体を取り付けることができる。
上述した本発明のグラファイト積層体およびグラファイト複合品は、主に電子機器の熱輸送用材料として、熱輸送用構造物に用いることができる。熱輸送用構造物とは、グラファイト積層体又はグラファイト複合品と、発熱素子と、を備え、グラファイト積層体又はグラファイト複合品は、発熱素子が発する熱によって昇温する部位である高温部位と、高温部位よりも温度が低い部位である低温部位とに接続されたものである。
(グラファイトシートの種類)
〔実施の形態C〕のグラファイトシートの種類に関しては、〔実施の形態B〕の(グラファイトシートの種類)の欄に記載の構成と同じ構成を採用することができる。
〔実施の形態C〕のグラファイトシートの製造方法に関しては、〔実施の形態B〕の(グラファイトシートの製造方法)の欄に記載の構成と同じ構成を採用することができる。
〔実施の形態C〕のグラファイトシートの面方向の熱伝導率に関しては、〔実施の形態B〕の(グラファイトシートの面方向の熱伝導率)の欄に記載の構成と同じ構成を採用することができる。
グラファイトシートの面方向の熱伝導率は、次式(1)によって算出した。
ここで、Aは、グラファイトシートの熱伝導率、αは、グラファイトシートの熱拡散率、dは、グラファイトシートの密度、Cpは、グラファイトシートの比熱容量をそれぞれ表わしている。なお、グラファイトシートの熱拡散率、密度、および比熱容量は、以下に述べる方法で求めた。
〔実施の形態C〕のグラファイトシートの厚さに関しては、〔実施の形態B〕の(グラファイトシートの厚さ)の欄に記載の構成と同じ構成を採用することができる。
(接着層材料の種類)
本発明における接着層の材料である接着層材料は、加熱によって接着性を発現するものが好ましく、熱硬化性樹脂、または、熱可塑性樹脂を用いることができる。
本発明における接着層材料の厚みは、特に限定されず、10μm未満が好ましい。更に具体的に、接着層材料の厚みは、0.1μm以上10μm未満が好ましく、1μm以上10μm未満がより好ましく、1μ以上9μm以下がより好ましく、1μm以上7μm以下がより好ましい。接着層材料の厚みが10μm未満であれば、接着層の熱伝導率は、グラファイトシートの熱伝導率に比べて、はるかに小さくなる。そのため、接着層材料の厚みを10μm未満に制御することで、グラファイトシート同士の間の伝熱を接着層によって阻害することなく良好に熱を伝達することができる。接着層材料の厚みが0.1μm以上(より好ましくは、1μm以上)であれば、接着層がグラファイトシート表面の凹凸を吸収しやすくなり、グラファイトシートと接着層との間の接触熱抵抗を低減することができ、効率的に熱を伝達することができる。また、接着層材料の厚みが0.1μm以上(より好ましくは、1μm以上)であれば、接着層が良好な接着性を示すことができる。また、上述した接着層材料の厚みであれば、グラファイト積層体の熱伝導率を、理論値に近い値にすることができる。接着層材料の厚みの算出方法は、後述する実施例にて説明したので、ここでは、その説明を省略する。
本発明における接着層の厚みは、接着層材料の厚みに比べて同じか、または、薄い。接着層が接着層材料よりも薄い場合、グラファイトシートの表面に接着層材料が浸潤している(グラファイトシート表面の凹凸を吸収している)と考えられる。具体的な接着層の厚みは、特に限定されず、10μm未満が好ましい。更に具体的に、接着層の厚みは、0.1μm以上10μm未満が好ましく、1μm以上10μm未満がより好ましく、1μ以上9μm以下がより好ましく、1μm以上7μm以下がより好ましい。接着層の厚みが10μm未満であれば、接着層の熱伝導率は、グラファイトシートの熱伝導率に比べて、はるかに小さくなる。そのため、接着層の厚みを10μm未満に制御することで、グラファイトシート同士の間の伝熱を接着層によって阻害することなく良好に熱を伝達することができる。接着層の厚みが0.1μm以上(より好ましくは、1μm以上)であれば、接着層がグラファイトシート表面の凹凸を吸収しやすくなり、グラファイトシートと接着層との間の接触熱抵抗を低減することができ、効率的に熱を伝達することができる。また、接着層が0.1μm以上(より好ましくは、1μm以上)あれば、良好な接着性を示すことができる。また、上述した接着層の厚みであれば、グラファイト積層体の熱伝導率を、理論値に近い値にすることができる。
(グラファイト積層体の製造方法の基本構成)
本発明のグラファイト積層体の製造方法は、グラファイトシートと接着層材料とを交互に積層して積層物を形成する積層工程と、積層物を加熱することによって、グラファイトシートと接着層とを熱融着させてグラファイト積層体を形成する接着工程と、を有する。さらに、グラファイト積層体の製造方法は、グラファイト積層体を切断処理する切断工程を有していてもよい。なお、本明細書において「熱融着」とは、樹脂またはワックスが加熱によって軟化して他の物質に接着することを意図する。
積層工程は、接着層の材料である接着層材料と、グラファイトシートとを交互に複数積層して積層物を形成する工程である。
接着工程は、積層工程にて形成された積層物を加熱することによって、接着層材料をグラファイトシートに熱融着させ、接着層と当該グラファイトシートとが交互に積層されたグラファイト積層体を得る工程である。加熱温度は、特に限定されず、接着層材料に応じて適宜選択できる。本工程中に、第1の加圧および第2の加圧を行う。第1の加圧および第2の加圧という2段階の加圧によって、積層物中のガスがよく抜けるので、平滑性とピール強度が高いグラファイト積層体を得ることができる。加熱温度、第1の加圧の圧力、第2の加圧の圧力としては、特に限定されず、接着層材料に応じて適宜選択することができる。なお、接着工程では、第2の加圧後に、第3の加圧、第4の加圧などの加圧をさらに1回以上行っても良い。また、接着工程では、第1の加圧と第2の加圧との間で、第3の加圧、第4の加圧などの加圧をさらに1回以上行っても良い。また、接着工程では、第1の加圧の前に、1回以上の予備加圧を行っても良い。但し、当該予備加圧にて積層物に加えられる圧力は、第1の加圧にて積層物に加える圧力、および、第2の加圧にて積層物に加える圧力よりも、低い圧力であることが好ましい。当該構成であれば、積層物中のガスが、更に良く抜ける。なお、第3の加圧、第4の加圧、および、予備加圧は、接着工程以外の工程で行うことも可能である。
実施の形態A~実施の形態Cにて説明したグラファイト積層体は、グラファイト積層体、保護層、粘着層から構成されるグラファイト複合フィルムとして構成することも可能である。
グラファイト積層体の周辺端部を保護層および粘着層で被覆した場合、保護層および粘着層が、グラファイト積層体からはみ出した構造となる。保護層のはみ出し幅は、2mm以下、好ましくは1mm以下である。はみ出し幅が2mm以下であれば、グラファイト積層体周辺の熱拡散に寄与しないはみ出し部分を小さくでき、省スペースの電子機器において、グラファイト積層体の面積を大きくする設計が可能となり、放熱特性に優れた電子機器を実現することができる。
(保護層の面積-グラファイト積層体の面積)/(グラファイト積層体の面積)で定義されるはみ出し面積の割合は50%以下、好ましくは30%以下、さらに好ましくは10%以下である。はみ出し面積の割合が50%以下であれば、グラファイト積層体周辺の熱拡散に寄与しないはみ出し部分を小さくでき、省スペースの電子機器において、グラファイト積層体の面積を大きくする設計が可能となり、放熱特性に優れた電子機器を実現することができる。
(グラファイト積層体の端部が被覆されている長さ)/(グラファイト積層体の端部長さ)で定義される被覆割合は10%以上、好ましくは20%以上、さらに好ましくは30%以上である。グラファイト積層体の端部の少なくとも一部分が保護層と粘着層とで被覆割合10%以上で被覆されたグラファイト複合フィルムであれば、グラファイト複合フィルムを剥離ライナーから引き剥がしたり、リワークしたりする際にグラファイト層間で凝集破壊することを防止することが可能になる。また、グラファイト複合フィルムを折り曲げた状態や繰り返し曲げた状態で使用しても、グラファイト複合フィルムの端部から層間剥離を起こしたり、保護層や粘着層とグラファイト積層体の界面から界面剥離を起こしたりせず、折り曲げや繰り返し曲げに耐えうる熱輸送用フィルムなる。
グラファイト複合フィルムの厚みは、100μm以下、好ましくは90μm、さらに好ましくは80μm以下である。厚み100μm以下のグラファイトフ複合フィルムであれば、グラファイト複合フィルムを引き剥がしたり、リワークしたり、折り曲げや繰り返し曲げ部に使用したりして、グラファイト複合フィルムに急な曲率で曲げの力が加わった場合でも、グラファイト層に余分な力が加わりにくくなり、グラファイトの層剥離がおこりにくくなる。
グラファイト複合フィルムの熱伝導率は、400W/m・K以上、好ましくは500W/m・K以上、さらに好ましくは600W/m・K以上である。熱伝導率が400W/m・K以上になると、熱伝導性が高いために、発熱機器から熱を逃がしやすくなり、発熱機器の温度上昇を抑えることが可能となる。ここで言う熱伝導率は、熱拡散率と熱容量と密度の積から算出した値である。
グラファイト複合フィルムのMIT(R1mm)は、100,000回以上、好ましくは200,000回以上、さらに好ましくは300,000回以上である。MIT(R1mm)が100,000回以上になると、グラファイト複合フィルムを、携帯電話のヒンジや小型電子機器の折り曲げ部分として好適に使用することができる。
保護層は、グラファイト積層体を取り扱ったり、電子機器に取り付けたりする際に、表面に傷や皺が入るのを保護するものである。またグラファイトは表面から黒鉛粉末が剥がれ落ちる場合があり、その粉落ちを防止するために、保護層を形成する。また、粘着層は、グラファイト積層体と、発熱部品、放熱部品、または、筐体等との密着をとるために使用され得る。
保護層および粘着層の各々の厚みは、40μm以下、好ましくは30μm以下、さらに好ましくは20μm以下である。保護層および粘着層に、各々、厚み40μm以下の保護層および粘着層を用いると、グラファイト複合フィルムを引き剥がしたり、リワークしたり、折り曲げや繰り返し曲げ部に使用したりして、グラファイト複合フィルムに急な曲率で曲げの力が加わった場合でも、グラファイト層に余分な力が加わりにくくなり、フィルムの層剥離がおこり難くなる。
保護層の具体例としては、絶縁層、および、導電層が挙げられる。絶縁層の材料としては、ポリイミド、ポリエチレンテレフタレート、および、エポキシ等が挙げられ、これらの材料は、耐熱性に優れ、グラファイト複合フィルムを発熱部品や放熱部品と複合化して使用した場合にも、十分な長期信頼性が得られる。
導電層の材料としては、銅、および、アルミニウム等が挙げられ、これら材料は、耐熱性に優れ、グラファイト複合フィルムを発熱部品や放熱部品と複合化して使用した場合にも、十分な長期信頼性が得られる。
粘着層の材料としては、アクリル系粘着材、および、シリコーン系粘着材等が挙げられ、これら材料は、耐熱性に優れ、グラファイト複合フィルムを発熱部品や放熱部品と複合化して使用した場合にも、十分な長期信頼性が得られる。また、取り付け位置の間違いや使用後の修理において、一度取り付けたグラファイト複合フィルムを取り外さなければならない場合がある。アクリル系粘着材、および、シリコーン系粘着材は、繰り返し使用や長期信頼性に優れるため、このような再利用性、および、再剥離性にも優れる。
上述したように、本発明のグラファイト積層体、熱輸送用構造物およびロッド状の熱輸送体は、曲がった形状を有し得る。当該形状を有していることは、本発明のグラファイト積層体、熱輸送用構造物およびロッド状の熱輸送体を様々な機器(例えば、電子機器または電気機器)に搭載した時に、当該機器の小型化を実現しつつ、かつ、当該機器の効率の良い放熱を実現するという観点から、有利である。この点について、図28を用いて説明する。
<熱伝導率の測定>
図23に示す測定装置を用いて下記の測定を行い、熱伝導率を算出した。
1)ロッド状の熱輸送体301の端部328を流水323(低温部位)と接触させて、20℃に保った。
2)ロッド状の熱輸送体301の端部327にヒーター322(高温部位)を取り付けた。熱電対325を端部327とロッド状の熱輸送体301とが接するところに取り付け、熱電対326を流水323と端部328とが接するところに取り付けた。熱電対325で測定される温度が高温部位の温度Tであり、熱電対326で測定される温度が、低温部位の温度(20℃)である。
3)ロッド状の熱輸送体301の低温部分以外を断熱材324で覆った。
4)高温部位が一定温度となるようにヒーター322の出力Qを調整した。
このとき、熱伝導率λは、ロッド状の熱輸送体301の断面Sと軸方向の長さLとをもちいて、
λ=Q×L/S(T-20℃)
との式に基づいて算出した。高温部位が100℃となるように調整したヒーター322の出力Qと、高温部位が50℃となるように調整したヒーター322の出力Qとを各々求め、高温部位が100℃のときの熱伝導率であるλa、および、高温部位が50℃のときの熱伝導率であるλbを求めた。
変形率は、下記手法により算出した。図26(1)に示すように、ロッド状の熱輸送体301が地面に平行となるようにして、ロッド状の熱輸送体301の両端部を第1クランプ312、第2クランプ313でそれぞれ保持した後、図26(2)に示すように、第2クランプ313の保持を外した。保持を外す前のロッド状の熱輸送体の端部の中心の位置と、保持を外した後で垂れ下がったロッド状の熱輸送体の端部の中心の位置と間の垂直距離x、および、ロッド状の熱輸送体の長さLを測定した。そして、x/Lを、ロッド状の熱輸送体の変形率とした。
高分子フィルム(ポリイミドフィルム)を熱処理して得られた、厚さ40μm、面方向熱伝導率1450W/mK、密度2.1g/cm3、電気伝導率14000S/cmのグラファイトシート(GS1と呼ぶ)を使用した。
200mm×200mmのサイズのグラファイトシートGS1とPETフィルム(厚み5μm、誘電率3.2、融点260℃)とを、交互に20枚積層し、当該積層体に対して、250℃に加熱されたプレス機を用いて0.5MPaの圧力を1分間付与して、積層体(厚み0.8mm)を得た。この積層体を切断し、2.7×0.8×90mmのロッド状の熱輸送体を作製した。
200mm×200mmのサイズのグラファイトシートGS1とPETフィルム(厚み5μm、誘電率3.2、融点260℃)とを、交互に68枚積層し、当該積層体に対して、250℃に加熱されたプレス機を用いて0.5MPaの圧力を1分間付与して、積層体(厚み2.7mm)を得た。この積層体を切断し、2.7×0.8×90mmのロッド状の熱輸送体を作製した。
200mm×200mmのサイズのグラファイトシートGS1とPETフィルム(厚み5μm、誘電率3.2、融点260℃)とを、交互に68枚積層し、当該積層体に対して、250℃に加熱されたプレス機を用いて0.5MPaの圧力を1分間付与して、積層体(厚み2.7mm)を得た。この積層体を切断し、2.7×2.7×90mmのロッド状の熱輸送体を作製した。
実施例3Aで得られたロッド状の熱輸送体を研磨し、当該熱輸送体の断面を直径2mmの円形(短軸も長軸も2mm)に加工することで、ロッド状の熱輸送体を作製した。
200mm×200mmのサイズのグラファイトシートGS1とPETフィルム(厚み5μm、誘電率3.2、融点260℃)とを、交互に20枚積層し、当該積層体に対して、250℃に加熱されたプレス機を用いて0.5MPaの圧力を1分間付与して、積層体(厚み0.8mm)を得た。この積層体を切断し、2.7×0.8×180mmのロッド状の熱輸送体を作製した。
グラファイトシートGS1の片面に、アクリル系両面テープ1(寺岡製作所(株)707:アクリル系13μm/PET4μm/アクリル系13μm)をラミネーターで貼り合せた。得られた粘着剤付きグラファイトフィルムを、同一方向に任意の形状に折り曲げながら、箱型に押し込んで張り合わせていく方法で、複数枚積層させ、プレス機により0.5MPaの圧力を1分間付与することにより、300mm×100mm×100mmのグラファイト直方体ブロックを作製した。この積層体を切断し、2.7×2.7×90mmのロッド状の熱輸送体を作製した。
NEC製スマートフォンMEDIAS X N-06Eに使用されているヒートパイプ(2.7×0.8×9.0mm)を取り外し、熱伝導率の測定を行った。
<B-1.グラファイトシート>
(グラファイトシートの基本構成)
実施例に用いたグラファイトシートの構成を、表1、および、以下に示す。
厚さゲージ(ハイデンハイン(株)社製、HElDENH:AIN-CERTO)を用い、50mm×50mmの形状に切り取られたグラファイトシートのサンプルについて、25℃の恒温室にて任意の10点における厚さを測定し、当該測定値の平均値として、グラファイトシートの厚さを算出した。
グラファイトシートの密度は、100mm×100mmの形状に切り取られたグラファイトシートのサンプルについて、重量および厚さを測定し、測定された重量の値を、算出された体積の値(100mm×100mm×厚さ)にて割ることにより、算出した。
グラファイトシートの電気伝導率は、4探針法で定電流を印加(例えば、(株)三菱化学アナリテック製ロレスタGP)することによって測定した。
グラファイトシートの面方向の熱伝導率は、次式(1)によって算出した。
ここで、Aは、グラファイトシートの熱伝導率、αは、グラファイトシートの熱拡散率、dは、グラファイトシートの密度、Cpは、グラファイトシートの比熱容量をそれぞれ表わしている。なお、グラファイトシートの熱拡散率、密度、および比熱容量は、以下に述べる方法で求めた。
グラファイトシートの表面粗さは、ミツトヨ製の小型表面粗さ測定器サーフテストSJ-210を用いて測定した。
(接着層の基本構成)
実施例に用いた接着層の構成を、表2、および、以下に示す。
接着層のガラス転移点は、示差走査熱量分析(島津製作所製DSC-50、昇温速度1℃/min)によって測定した。
厚さゲージ(ハイデンハイン(株)社製、HElDENH:AIN-CERTO)を用い、50mm×50mmの形状に切り取られた接着層のサンプルについて、25℃の恒温室にて任意の10点における厚さを測定し、当該測定値の平均値として、接着層の厚さを算出した。
接着層の誘電率は、接着層の誘電率は、温度20℃および湿度60%の条件で24時間放置後、安藤電気(株)製AS-4245を用いて、周波数1kHzで測定した。
接着層の吸水率は、JIS K 7209に準拠し、乾燥状態の接着層の質量と、水に24時間浸漬した後の接着層の質量とを比較することによって測定した。
接着層のアウトガスの有無は、試料を150℃まで加熱したときのガスをガスクロマトグラフィーで確認することによって確認した。
TENSILON UTM-2(エー・アンド・デイ社製)を用い、フィルムを3mm×35mmに切り出して、当該フィルムを治具に固定し、チャック間距離20mmになり、かつ、フィルムの中心が引張試験機の中心と重なるように、上記治具を引張試験機にセットし、クロスヘッドスピード8mm/minで引張り試験を行い、接着層の破断強度の測定を行った。
接着層の接着力は、JIS-Z0237記載の方法1の「試験板に対する180度引きはがし粘着力の試験方法」に準じて求めた。JIS-Z0237記載の幅50mm×長さ125mm×厚さ1.1mm、表面粗さRa:50nmのSUS板をメタノールで洗浄した。20mm×300mmの保護層を、環境温度23℃、湿度50%の条件下において、2kgのローラーで洗浄後のSUS板に空気が入らないように2往復加圧貼付した。1時間放置後、SIMAZU製のオートグラフ(型番:AG-10TB)、50Nのロードセル(型番:SBL-50N)を用い、同一の温度湿度条件下で300mm/minの速度で引っ張って、180度引きはがし粘着力を測定した。3回測定した値の平均値を、小数点以下第3位を四捨五入して小数点以下第2位まで、N/25mmの単位で算出した。
(比較例1B、3B、5B、7B、参考例1B、2Bのグラファイト積層体の製造方法)
200mm×300mmのサイズ(厚さは、表1に記載)の表1に記載のグラファイトシートの片面に、表2に記載の接着層を、ラミネーターを用いて貼り合せた。
200mm×300mmのサイズ(厚さは、表1に記載)の表1に記載のグラファイトシートと表2に記載の接着層とを、交互に表3に記載の数だけ積層し、当該積層体に対して、180℃に加熱されたプレス機を用いて0.5MPaの圧力を1分間付与し、これによって、二軸方向にグラファイト結晶が配向したグラファイトブロックを得た。
表1に記載のグラファイトシートの片面に、十条ケミカル製ポリエステル系接着剤を、乾燥後の厚さが3μmになるように塗工し、接着層付きグラファイトシートを作製した。
表1に記載のグラファイトシートと表2に記載の接着層とを、交互に表3に記載の数だけ積層し、当該積層体に対して、250℃に加熱されたプレス機を用いて0.5MPaの圧力を1分間付与し、これによって、二軸方向にグラファイト結晶が配向したグラファイトブロックを得た。
グラファイトフィルムに溶液状のポリイミド前駆体(東レ(株)製トレニース)を10μmの厚さに塗布した。そして、減圧乾燥の後、まだ十分にイミド化が進行していないフィルム20枚を積層し、加熱圧着を行って、グラファイト積層体を得た。加熱圧着において、温度は300℃であり、圧力は10Kg/cm2であった。
縦横約50mm、厚さ約0.1mm、面内方向熱伝導率600W/mKのグラファイトシートと、縦横約50mm、厚さ約0.4mmのゴムシート(EPDMからなるゴムシート、弾性率1.7MPa)とを用いて、グラファイト積層体を作製した。
実施例2において、熱プレス後の積層体を、NCカッターにて、図17の形状に切断し、90mm(積層方向に垂直な面の長辺方向)×2.75mm(積層方向に垂直な面の短辺方向)×0.8mm(積層方向)の屈曲部を有するグラファイト積層体を得た。
実施例2において、熱プレス時に図6のように屈曲を有する金型を用いて熱プレスをおこなった後、シングルワイヤーソーで積層方向に垂直に切断し、図18のように、90mm(積層方向に垂直な面の長辺方向)×0.8mm(積層方向に垂直な面の短辺方向)×2.75mm(積層方向)の屈曲部を有するグラファイト積層体を得た。
厚さゲージ(ハイデンハイン(株)社製、HElDENH:AIN-CERTO)を用い、50mm×50mmの形状に切り取られたグラファイトシートのサンプルについて、25℃の恒温室にて任意の10点における厚さを測定し、当該測定値の平均値として、グラファイト積層体の厚さを算出した。
グラファイト積層体の材料であるグラファイトシートの厚さをA1[μm]とし、積層数をB1[枚]とする。一方、グラファイト積層体の材料である接着層の厚さをA2[μm]とし、積層数をB2[枚]とする。
Y=X÷(A1×B1+A2×B2)
上記の式にしたがって、Yを算出した。
グラファイト積層体の面方向の熱伝導率は、次式(2)によって算出することができる。
ここで、A1は、グラファイト積層体の熱伝導率、α1は、グラファイト積層体の熱拡散率、d1は、グラファイト積層体の密度、Cp1は、グラファイト積層体の比熱容量をそれぞれ表わしている。なお、グラファイト積層体の熱拡散率、密度、および比熱容量は、以下に述べる方法で求めることができる。
グラファイト積層体の熱伝導率(理論値)は、「グラファイトシートの熱伝導率×グラファイトシートの厚みの合計÷積層体の厚み」によって算出した。
グラファイト積層体の熱伝導率(理論値との近さ)は、「熱伝導率の実測値÷熱伝導率(理論値)」によって算出した。
グラファイト積層体の積層作業性は、目視にて判定した。
グラファイト積層体への泡のかみ込みは、目視にて判定した。
グラファイト積層体の切断性は、目視にて判定した。
グラファイト積層体が地面に対して水平になるようにグラファイト積層体の端部の1つを固定した後、固定した端部から4cm離れたグラファイト積層体の表面にマーキングを施した。当該マーキングを施した箇所に対して、マーキングを施した箇所におけるグラファイト積層体の断面1mm2あたり0.7gの荷重をかけた。荷重をかける前のマーカーの位置と、荷重をかけた後のマーカーの位置との間の距離(変位)を測定した。
W(g)=[サンプルの幅(mm)]×[サンプルの厚さ(mm)]×0.7(g)
=16×L×0.7
なお、上記式の「L」には、表3に記載の「厚さ(mm)」の値を代入すればよい。
実施例では、「熱伝導率(理論値との近さ)」、「積層作業性」、「泡かみ込み性」および「切断性」の何れにおいても優れていることが明らかになった。
<C-1.グラファイトシート>
(グラファイトシートの基本構成)
実施例に用いたグラファイトシートは、高分子フィルム(ポリイミドフィルム)を熱処理して得られた、厚み40μm、幅210mm、長さ260mm、面方向熱伝導率1300W/mKのグラファイトシートであった。
厚みゲージ(ハイデンハイン(株)社製、HElDENH:AIN-CERTO)を用い、50mm×50mmの形状に切り取られたグラファイトシートのサンプルについて、25℃の恒温室内にて任意の10点における厚みを測定し、当該測定値の平均値として、グラファイトシートの厚みを算出した。
(接着層の基本構成)
実施例に用いた接着層材料は、PET(polyethylene terephthalate、融点260℃)であった。また、各物性の測定方法を以下に説明する。
接着層の融解温度は、JIS K 7121に準拠し、示差走査熱量分析装置(島津製作所製DSC-50)によって測定した。
(実施例1C~11C、参考例1C~11Cのグラファイト積層体の製造方法)
グラファイトシートと接着層材料とを、交互に表4に記載の数だけ積層して積層物を作製した。次に、表4に記載の所定の温度のときに所定の圧力を所定の時間、積層物に対して付与し、二軸方向にグラファイト結晶が配向したグラファイト積層体を得た。なお第2の加圧を行う場合は、第1の加圧の後で第2の加圧を行った。
グラファイトシートと接着層材料とを、表5に記載の数だけ交互に積層して積層物を作製した。この積層物を表5に記載の段数だけ積層した。次に、表5に記載の所定の温度のときに所定の圧力を所定の時間、積層物に対して付与し、二軸方向にグラファイト結晶が配向したグラファイト積層体を得た。なお第2の加圧を行う場合は、第1の加圧の後で第2の加圧を行った。
グラファイト積層体のピール強度を判定するにあたり、まず、刃角が30度のセンター刃であるトムソン刃と50トンプレス機によって、幅210mm、長さ260mmのグラファイト積層体の面内5点(左上、左下、真ん中、右上、右下)で抜き加工し、幅210mm、長さ64mmのグラファイト積層体を5つ得た。得られたグラファイト積層体について、グラファイトシートと接着層との層間での剥がれの有無を目視にて確認した。得られた5つのグラファイト積層体について、全て剥がれが無い場合を「3」、1つから2つ剥がれた場合を「2」、3つ以上剥がれた場合を「1」と判定した。
グラファイト積層体のSEM画像から、接着層とグラファイトシートとの界面の断面を確認し、接着層とグラファイトシートとが接着している部分の長さを、界面全体の長さで割り、接着割合を算出した。SEM画像の観察は、超高分解能走査型電子顕微鏡観察(FE-SEM)で行い、装置としてULTRAplus(CarlZeiss製)を用い、加速電圧が5.0kVの条件で、二次電子検出器SE2で試料を観察した。また、グラファイト積層体を樹脂包埋させた後、当該包埋物をCP(クロスセクションポリッシャー)によって処理することにより、観察対象である断面を有する試料を作製した。
図22に示す測定装置を用いて下記の測定を行い、熱の伝わり易さ(ヒーター部と冷却部の温度差)を算出した。グラファイト積層体201の端部211を流水203(低温部位)と接触させて、18℃に保った。グラファイト積層体201の端部209にヒーター202(高温部位)を取り付けた。熱電対207を端部209とグラファイト積層体201とが接するところに取り付けた。グラファイト積層体201の低温部分以外を断熱材204で覆った。ヒーター202の出力を2Wに調整した。測定したヒーター部の温度と冷却部の温度との差を確認することで、熱の伝わり易さを算出した。熱の伝わり易さは、その値が低いほど熱が伝わり易いと判断した。
厚みゲージ(ハイデンハイン(株)社製、HElDENH:AIN-CERTO)を用い、50mm×50mmの形状に切り取られたグラファイト積層体のサンプルについて、25℃の恒温室内にて任意の9点における厚みを測定し、当該測定値の平均値として、グラファイト積層体の厚みおよび厚み誤差を算出した。
上記の測定した9点の厚みから、厚みの最大値と最小値との平均値を中心値として、中心値とどのくらいの割合で厚みがばらつくのかを算出した。厚み誤差が±5%以内の場合を「5」、厚み誤差が5%以上10%以下の場合を「4」、厚み誤差が10%以上15%以下の場合を「3」、厚み誤差が15%以上20%以下の場合を「2」、厚み誤差が20%以上30%以下の場合を「1」と判定した。
グラファイト積層体の外観は、グラファイト積層体内への泡のかみ込みを目視にて判定し、その結果に基づいて評価した。泡によってグラファイト積層体が変形している場合を「1」と判定し、グラファイト積層体の内部全体に泡が入っている場合を「2」と判定し、グラファイト積層体の内部の一部に泡が入っている場合を「3」と判定し、グラファイト積層体の内部に泡が入っていない場合を「4」と判定した。
グラファイトシートの積層数が同じもの同士を比較すると、実施例は参考例に比べて、「ピール強度」、「熱の伝わり易さ」、「平滑性」および「外観」の何れにおいても優れていた。
5 グラファイトシート
6 接着層
7 積層面
10 屈曲部(第1の屈曲部)
11 屈曲部(第2の屈曲部)
12 屈曲部(第3の屈曲部)
15 領域
16 領域
17 領域
30 加圧治具
50 接着部
51 未接着部
100 発熱素子
101 金属板
102 伝熱材料
110 側面図
120 上面図
201 グラファイト積層体
202 ヒーター
203 流水
204 断熱材
205 グラファイトシート
206 接着層
207 熱電対(高温部位温度測定)
208 熱電対(低温部位温度測定)
209 端部(高温部位に接触)
210 屈曲部
211 端部(低温部位に接触)
235 切断箇所
301 ロッド状の熱輸送体
302 第1CPU
303 プレート
304 ケース
305 第2CPU
312 第1クランプ
313 第2クランプ
322 ヒーター
323 流水
324 断熱材
325 熱電対
326 熱電対
327 端部
328 端部
401 グラファイト積層体
402 粘着層
403 保護層
501 グラファイト積層体
540 高温部位
541 低温部位
550 電子部品
601 ロッド状の熱輸送体
Claims (31)
- ロッド状の熱輸送体であって、該ロッド状の熱輸送体は、熱輸送体の一方の端部を高温部位に接触させ、かつ、他方の端部を20℃に保たれた低温部位に接触させて測定される熱伝導率が、式(1)の関係を満足するロッド状の熱輸送体。
λa/λb>0.7 式(1)
式(1)において、λaは、上記高温部位の温度が100℃であるときの熱伝導率を表し、λbは上記高温部位の温度が50℃であるときの熱伝導率を表す。 - 上記ロッド状の熱輸送体は、グラファイトを含む請求項1に記載のロッド状の熱輸送体。
- 上記ロッド状の熱輸送体は、層状構造を有していることを特徴とする請求項2に記載のロッド状の熱輸送体。
- ロッド状の熱輸送体であって、該ロッド状の熱輸送体は、グラファイトシートと接着層とが交互に積層されてなり、上記グラファイトシートの積層数が、3層以上500層以下であることを特徴とするロッド状の熱輸送体。
- 上記ロッド状の熱輸送体は、該ロッド状の熱輸送体の断面の短軸aと長軸bとの比a/bが1/500以上のものであることを特徴とする請求項1~4のいずれか1項に記載のロッド状の熱輸送体。
- 上記ロッド状の熱輸送体は、ロッド長さLが4cm以上のものであることを特徴とする請求項1~5のいずれか1項に記載のロッド状の熱輸送体。
- 上記ロッド状の熱輸送体は、該熱輸送体が地面に対して水平になるように該熱輸送体の両端部を保持した後、一方の端部の保持を外した場合に、保持が外された端部の中心の位置が、ロッドの長さLの10%以下だけ、保持が外される前の位置から垂直に下方へ変化するものであることを特徴とする請求項1~6のいずれか1項に記載のロッド状の熱輸送体。
- ヒートパイプとして用いられるものである請求項1~7のいずれか1項に記載のロッド状の熱輸送体。
- 電子機器内部に組み込まれて用いるロッド状の熱輸送体であって、該熱輸送体は、グラファイト成分を含むものであり、かつ、熱輸送体の一端は発熱体に接続され、他方の一端は発熱体よりも低温である低温部位に接続されて、サーマルハイウエイとして用いられるものであることを特徴とするロッド状の熱輸送体。
- 発熱体と、発熱体よりも低温である低温部と、サーマルハイウエイと、を備える電子機器であって、上記サーマルハイウエイが請求項1~9のいずれか1項に記載のロッド状の熱輸送体であることを特徴とする電子機器。
- 交互に積層されているグラファイトシートと接着層とを含むグラファイト積層体であって、
上記接着層は、熱可塑性樹脂および熱硬化性樹脂のうちの少なくとも1つの樹脂を含むものであり、
上記接着層は、吸水率が2%以下のものであり、かつ、厚さが15μm未満のものであり、
上記グラファイト積層体に含まれる上記グラファイトシートの積層数が、3層以上であることを特徴とする、グラファイト積層体。 - 交互に積層されているグラファイトシートと接着層とを含むグラファイト積層体であって、
上記接着層は、熱可塑性樹脂および熱硬化性樹脂のうちの少なくとも1つの樹脂を含むものであり、
上記接着層は、厚さが15μm未満のものであり、
上記グラファイト積層体に含まれる上記グラファイトシートの積層数が、3層以上であり、
上記グラファイト積層体の吸水率が0.25%以下であることを特徴とする、グラファイト積層体。 - 上記熱可塑性樹脂および上記熱硬化性樹脂は、ガラス転移点が50℃以上のものであることを特徴とする、請求項11または12に記載のグラファイト積層体。
- 上記グラファイトシートは、面方向の熱伝導率が1000W/(m・K)以上のものであることを特徴とする、請求項11~13の何れか1項に記載のグラファイト積層体。
- 上記グラファイト積層体は、当該グラファイト積層体の少なくとも1つ以上の屈曲部において折り曲げられた形状を有していることを特徴とする、請求項11~14の何れか1項に記載のグラファイト積層体。
- X軸と当該X軸に直交するY軸とによって規定される表面を有する、グラファイトシートおよび接着層が、上記表面を重ねた状態にて、上記表面と垂直に交わるZ軸の方向に向かって交互に積層されてなるグラファイト積層体であって、
上記グラファイト積層体は、当該グラファイト積層体の少なくとも2つ以上の屈曲部において折れ曲げられた形状を有しており、
上記屈曲部の各々は、以下の(a)~(c)の何れかであることを特徴とする、グラファイト積層体:
(a)上記グラファイト積層体を、上記X軸の方向または上記Y軸の方向に向かって屈曲させた第1の屈曲部、
(b)上記グラファイト積層体を、上記Z軸の方向に向かって屈曲させた第2の屈曲部、
(c)上記グラファイト積層体を、上記X軸の方向または上記Y軸の方向に向かって屈曲させ、かつ、上記Z軸の方向に向かって屈曲させた第3の屈曲部。 - X軸と当該X軸に直交するY軸とによって規定される表面を有する、グラファイトシートおよび接着層が、上記表面を重ねた状態にて、上記表面と垂直に交わるZ軸の方向に向かって交互に積層されてなるグラファイト積層体であって、
上記グラファイト積層体は、当該グラファイト積層体の少なくとも1つ以上の屈曲部において折れ曲げられた形状を有しており、
上記屈曲部の各々は、以下の(c)であることを特徴とする、グラファイト積層体:
(c)上記グラファイト積層体を、上記X軸の方向または上記Y軸の方向に向かって屈曲させ、かつ、上記Z軸の方向に向かって屈曲させた第3の屈曲部。 - 上記グラファイト積層体は、上記グラファイト積層体が地面に対して水平になるように上記グラファイト積層体の一方の端部を固定した後、固定した上記端部から4cm離れた位置における上記グラファイト積層体の断面に対して、当該断面1mm2あたり0.7gの荷重をかけたときに、上記断面の変位が15mm以下のものであることを特徴とする、請求項11~17の何れか1項に記載のグラファイト積層体。
- 請求項11~18の何れか1項に記載のグラファイト積層体と、発熱素子と、を備えている熱輸送用構造物であって、
上記グラファイト積層体は、上記発熱素子が発する熱によって昇温する部位である高温部位と、上記高温部位よりも温度が低い部位である低温部位とに接続されていることを特徴とする、熱輸送用構造物。 - 交互に積層されているグラファイトシートと接着層とを含むグラファイト積層体の製造方法であって、
上記グラファイトシートと上記接着層とを交互に積層して積層物を形成する積層工程と、
上記積層物を、加圧することによって、または、加熱および加圧することによって、上記グラファイトシートと接着層とを接着させて上記グラファイト積層体を形成する接着工程と、を有することを特徴とする、グラファイト積層体の製造方法。 - 上記接着層は、熱可塑性樹脂および熱硬化性樹脂のうちの少なくとも1つの樹脂を含むものであり、かつ、吸水率が2%以下のものであることを特徴とする、請求項20に記載のグラファイト積層体の製造方法。
- 上記接着層は、25℃での接着力が1N/25mm以下のものであることを特徴とする、請求項20または21に記載のグラファイト積層体の製造方法。
- 上記接着工程は、上記グラファイト積層体を折り曲げる少なくとも1つ以上の屈曲部を有するグラファイト積層体を形成する屈曲部形成工程を包含することを特徴とする、請求項20~22の何れか1項に記載のグラファイト積層体の製造方法。
- 上記積層工程は、X軸と当該X軸に直交するY軸とによって規定される表面を有する、上記グラファイトシートおよび上記接着層を、上記表面を重ねた状態にて、上記表面と垂直に交わるZ軸の方向に向かって交互に積層させて上記積層物を形成する工程を包含し、
上記屈曲部形成工程は、2つ以上の屈曲部を有するグラファイト積層体を形成する、以下の(d)~(h)の屈曲部形成工程の少なくとも1つを包含することを特徴とする、請求項23に記載のグラファイト積層体の製造方法:
(d)加熱および加圧された上記積層物を上記Z軸の方向に切断して、上記積層物から上記グラファイト積層体を切り出すことにより、上記グラファイト積層体に、上記X軸の方向または上記Y軸の方向に向かって屈曲した第1の屈曲部を形成する、第1の屈曲部形成工程、
(e)屈曲した形状を有する加圧治具によって、加熱および加圧された上記積層物を加圧することにより、上記グラファイト積層体に、上記Z軸の方向に向かって屈曲した第2の屈曲部を形成する、第2の屈曲部形成工程、
(f)屈曲した形状を有する加圧治具によって、加熱および加圧された上記積層物を加圧して、当該積層物をZ軸の方向に向かって屈曲させた後で、当該積層物を上記Z軸の方向に切断して、当該積層物から上記グラファイト積層体を切り出すことにより、上記グラファイト積層体に、上記Z軸の方向に向かって屈曲した第2の屈曲部を形成する、第3の屈曲部形成工程、
(g)加熱および加圧された上記積層物を上記Z軸の方向に切断して、上記積層物から、上記X軸の方向または上記Y軸の方向に向かって屈曲したグラファイト積層体の前駆体を切り出した後で、屈曲した形状を有する加圧治具によって、当該グラファイト積層体の前駆体を加圧することにより、上記グラファイト積層体に、上記X軸の方向または上記Y軸の方向に向かって屈曲し、かつ、上記Z軸の方向に向かって屈曲した第3の屈曲部を形成する、第4の屈曲部形成工程、
(h)屈曲した形状を有する加圧治具によって、加熱および加圧された上記積層物を加圧して、当該積層物をZ軸の方向に向かって屈曲させた後で、当該積層物を上記Z軸の方向に対して斜めに切断して、当該積層物から上記グラファイト積層体を切り出すことにより、上記グラファイト積層体に、上記X軸の方向または上記Y軸の方向に向かって屈曲し、かつ、上記Z軸の方向に向かって屈曲した第3の屈曲部を形成する、第5の屈曲部形成工程。 - 上記積層工程は、X軸と当該X軸に直交するY軸とによって規定される表面を有する、上記グラファイトシートおよび上記接着層を、上記表面を重ねた状態にて、上記表面と垂直に交わるZ軸の方向に向かって交互に積層させて上記積層物を形成する工程を包含し、
上記屈曲部形成工程は、1つ以上の屈曲部を有するグラファイト積層体を形成する、以下の(g)および(h)の屈曲部形成工程の少なくとも1つを包含することを特徴とする、請求項23に記載のグラファイト積層体の製造方法:
(g)加熱および加圧された上記積層物を上記Z軸の方向に切断して、上記積層物から、上記X軸の方向または上記Y軸の方向に向かって屈曲したグラファイト積層体の前駆体を切り出した後で、屈曲した形状を有する加圧治具によって、当該グラファイト積層体の前駆体を加圧することにより、上記グラファイト積層体に、上記X軸の方向または上記Y軸の方向に向かって屈曲し、かつ、上記Z軸の方向に向かって屈曲した第3の屈曲部を形成する、第4の屈曲部形成工程、
(h)屈曲した形状を有する加圧治具によって、加熱および加圧された上記積層物を加圧して、当該積層物をZ軸の方向に向かって屈曲させた後で、当該積層物を上記Z軸の方向に対して斜めに切断して、当該積層物から上記グラファイト積層体を切り出すことにより、上記グラファイト積層体に、上記X軸の方向または上記Y軸の方向に向かって屈曲し、かつ、上記Z軸の方向に向かって屈曲した第3の屈曲部を形成する、第5の屈曲部形成工程。 - 交互に積層されているグラファイトシートと接着層とを含むグラファイト積層体であって、
上記接着層は、熱可塑性樹脂および熱硬化性樹脂のうちの少なくとも1つの樹脂を含むものであり、
上記グラファイト積層体に含まれる上記グラファイトシートの積層数が、3層以上であり、
上記グラファイトシートと上記接着層とは、界面の50%以上において、互いに密着しているグラファイト積層体。 - 接着層の材料である接着層材料と、グラファイトシートとを交互に複数積層して積層物を得る積層工程と、
上記積層物を加熱して、上記接着層材料を上記グラファイトシートに熱融着させ、上記接着層と当該グラファイトシートとが交互に積層されたグラファイト積層体を得る接着工程と、を備えるグラファイト積層体の製造方法であって、
上記接着層材料は、熱可塑性樹脂および熱硬化性樹脂のうちの少なくとも1つの樹脂を含むものであり、
上記接着工程では、上記接着層材料の温度が[(接着層材料の融解温度)-20℃]に到達するまでに少なくとも、上記積層物を加圧する第1の加圧を行い、
上記第1の加圧では、上記接着層材料が上記グラファイトシートに熱融着しないように上記積層物を加圧し、
さらに上記接着工程では、上記接着層材料の温度が[(接着層材料の融解温度)-20℃]以上になった後に少なくとも、上記積層物を加圧する第2の加圧を行い、
上記第2の加圧では、上記接着層材料が上記グラファイトシートに熱融着するように上記積層物を加圧するグラファイト積層体の製造方法。 - 上記第2の加圧では、上記第1の加圧よりも、高い圧力で上記積層物を加圧する請求項27に記載のグラファイト積層体の製造方法。
- 上記第2の加圧では、上記第1の加圧よりも、高い圧力および高い温度で上記積層物を加圧する請求項27に記載のグラファイト積層体の製造方法。
- 上記接着工程の開始時点から、上記第1の加圧を行う請求項27~29の何れか1項に記載のグラファイト積層体の製造方法。
- 接着層の材料である接着層材料と、グラファイトシートとを交互に複数積層して積層物を得る積層工程と、
上記積層物を加熱して、上記接着層材料を上記グラファイトシートに熱融着させ、上記接着層と当該グラファイトシートとが交互に積層されたグラファイト積層体を得る接着工程と、を備えるグラファイト積層体の製造方法であって、
上記接着層材料は、熱可塑性樹脂および熱硬化性樹脂のうちの少なくとも1つの樹脂を含むものであり、
上記積層工程では、上記積層物を複数積層させるグラファイト積層体の製造方法。
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Also Published As
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CN107148669A (zh) | 2017-09-08 |
JP2018195828A (ja) | 2018-12-06 |
CN110065272B (zh) | 2021-06-11 |
JP6360198B2 (ja) | 2018-07-18 |
JPWO2016098890A1 (ja) | 2017-10-19 |
KR20170095316A (ko) | 2017-08-22 |
CN110065272A (zh) | 2019-07-30 |
US20180023904A1 (en) | 2018-01-25 |
CN107148669B (zh) | 2020-04-07 |
KR102087163B1 (ko) | 2020-03-10 |
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