CN109796759B - Cyanate ester-based carbon fiber composite material with high thermal conductivity coefficient and preparation method thereof - Google Patents
Cyanate ester-based carbon fiber composite material with high thermal conductivity coefficient and preparation method thereof Download PDFInfo
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Abstract
The invention relates to the technical field of resin matrix composite materials, and particularly discloses a cyanate ester-based carbon fiber composite material with a high thermal conductivity coefficient for a space optical structure and a preparation method thereof. The composite material comprises a cyanate/carbon fiber composite material main body and a high-thermal-conductivity functional layer, wherein the high-thermal-conductivity functional layer covers the cyanate/carbon fiber composite material main body. The composite material comprises a cyanate ester/carbon fiber composite material main body and a high-thermal-conductivity functional layer, wherein the high-thermal-conductivity filler content in the high-thermal-conductivity functional layer is high and consistent with a matrix of the cyanate ester/carbon fiber composite material main body, so that the interface problem is avoided, the temperature uniformity of a sensor and the like can be improved when the composite material is used for a space optical structure, and the composite material has important significance for improving the temperature gradient of a low-thermal-conductivity structural member on a space optical remote sensor.
Description
Technical Field
The invention relates to the technical field of resin matrix composite materials, in particular to a high-thermal-conductivity cyanate ester-based carbon fiber composite material for a space optical structure and a preparation method thereof.
Background
High-performance composite materials have an indispensable position in the aerospace field, and support the development of aerospace industry together with steel, titanium alloy and aluminum alloy. The high-strength high-toughness high-strength light-weight high-modulus high-toughness high-strength high-corrosion-resistance high-weather-resistance high-performance high-strength high-toughness high-corrosion-resistance high-weather-resistance high-performance high-toughness high-corrosion-resistance high-weather-resistance high-performance high-toughness high-performance high-. However, devices applied to the aerospace and military fields generally need to operate in harsh environments, such as high frequency, high power, high pressure, high temperature and the like, and are required to have high reliability, long safety and extremely high heat dissipation requirements. Therefore, higher requirements are also placed on the thermal conductivity of the polymer composite. In order to maintain the position of the polymer composite material, it has been studied that the composite material has excellent overall properties, and particularly, has high thermal conductivity.
An economical and effective way to increase the thermal conductivity of polymers is to add thermally conductive fillers. By filling the heat-conducting filler, the heat conductivity of the polymer can be greatly improved, and the polymer composite material with different heat-conducting performance requirements can be prepared. CN102766309A discloses a formula of a filled modified polytetrafluoroethylene high-thermal-conductivity composite material and an acquisition method thereof, wherein the volume fraction of graphite filling is 18 +/-0.5%, and the volume fraction of carbon fiber filling is 10%. However, the main problem of the filled polymer-based heat conduction material is that the thermal conductivity of the composite material is improved along with the increase of the content of the thermal conductive filler, and the mechanical property of the material is inevitably deteriorated. Therefore, in order to make the heat conductive material practically applicable, the heat conductive performance of the composite material is often reduced, which inevitably limits the heat conductive performance and the use performance of the heat conductive material.
The conduction of heat in the composite material depends on the formation of phonon heat conduction channels, and inevitably passes through a plurality of interfaces of polymers and fillers, so that the interface bonding strength between the polymers and the fillers is increased, and the heat conduction performance of the composite material is improved. However, the compatibility between the interface of the inorganic filler particles and the polymer resin matrix is poor, the filler particles are difficult to be uniformly dispersed in the resin matrix and are easy to form agglomeration, and meanwhile, the difference of the surface tension of the inorganic filler particles and the polymer resin matrix causes gaps to exist in the interface, so that the thermal resistance of the interface can not be effectively reduced, and the interface effect is more obvious after the inorganic filler particles and the carbon fibers form a composite material.
Disclosure of Invention
The invention aims to overcome the technical problems that the high-thermal-conductivity composite material prepared by a filling method in the prior art is easy to agglomerate, the filling amount is low due to poor interface compatibility, and the thermal conductivity and the service performance are further influenced, and provides a novel high-thermal-conductivity cyanate-based carbon fiber composite material for a space optical structure and a preparation method thereof.
In order to achieve the purpose, the invention adopts the following technical scheme:
in one aspect, the invention provides a cyanate ester-based carbon fiber composite material with high thermal conductivity for a space optical structure, which comprises a cyanate ester/carbon fiber composite material main body and a high thermal conductivity functional layer, wherein the high thermal conductivity functional layer covers the cyanate ester/carbon fiber composite material main body.
In some embodiments, the composite material is obtained by integrally curing and molding the cyanate ester/carbon fiber composite material main body and the high thermal conductivity functional layer.
In some embodiments, the high thermal conductivity functional layer has a thermal conductivity of 0.5W/(m.K) to 2W/(m.K).
In some embodiments, the high thermal conductivity functional layer is obtained by laying one or more layers of high thermal conductivity cyanate ester/carbon fiber prepregs on the cyanate ester/carbon fiber composite material main body according to a certain laying angle.
In some embodiments, the reinforcing material of the high thermal conductivity cyanate/carbon fiber prepreg is one or more of carbon fibers with a thermal conductivity of 30W/(m · K) to 200W/(m · K).
In some embodiments, the resin matrix of the high thermal conductivity cyanate/carbon fiber prepreg is a cyanate resin in which a high thermal conductivity filler is uniformly dispersed.
In some embodiments, the high thermal conductivity filler is selected from at least one of graphite, alumina, magnesia, silicon carbide, or carbon nanotubes.
In some embodiments, the high thermal conductivity filler is 30 to 50% by mass based on 100% by mass of the high thermal conductivity functional layer.
In still another aspect, the present invention provides a preparation method of the above composite material, including: s1, according to the layering angle and sequence, laying cyanate/carbon fiber prepreg on a mould to obtain a cyanate/carbon fiber composite material main body, and laying a high-thermal-conductivity functional layer with a certain angle on the topmost layer of the cyanate/carbon fiber composite material main body; and S2, putting the whole body into a furnace, curing and compression molding to obtain the composite material.
In some embodiments, the high thermal conductive functional layer is prepared by laying a prepreg obtained by coating a cyanate ester resin adhesive solution of an ultrasonically dispersed high thermal conductive filler and hot-melting and pre-dipping carbon fibers.
The invention has the beneficial effects that: the high-thermal conductivity coefficient composite material comprises a cyanate/carbon fiber composite material main body and a high-thermal conductivity functional layer, wherein the high-thermal conductivity filler content in the high-thermal conductivity functional layer is high and is consistent with a matrix of the cyanate/carbon fiber composite material main body, so that the interface problem is avoided; the composite material main body can also be obtained by hot-melting and pre-dipping the resin film with uniformly dispersed fillers and the carbon fibers, and the composite material main body and the fillers with high content in the outer functional layer act together, so that the defects of low filling amount, poor heat conduction effect and influence on other properties in a pure filling method are overcome, and the composite material main body has excellent heat conduction effect and can ensure that other properties are still good; the composite material can be used for space optical structures, can improve the temperature uniformity of sensors and the like, and has important significance for improving the temperature gradient of low-thermal-conductivity structural members on space optical remote sensors.
In the composite material, the high heat conduction layer is obtained by adopting a prepreg laying process to be combined with the composite material main body and then integrally curing and forming, the requirements of the complex process and equipment of a coating method are different, the interface integration combination is realized by fewer steps, the process is simple, and the industrial production is easy.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is further described in detail with reference to the following embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not to be construed as limiting the invention.
The invention provides a cyanate ester carbon fiber composite material with high thermal conductivity, which comprises a cyanate ester/carbon fiber composite material main body and a high thermal conductivity functional layer, wherein the high thermal conductivity functional layer covers the cyanate ester/carbon fiber composite material main body. Specifically, the composite material is obtained by integrally curing and molding a cyanate ester/carbon fiber composite material main body and a high-thermal-conductivity functional layer. The composite material can be used in space optical structures.
The high-thermal-conductivity functional layer is obtained by laying one or more layers of cyanate ester/carbon fiber prepreg with high thermal conductivity on a cyanate ester/carbon fiber composite material main body according to a certain laying angle. The heat conductivity coefficient of the high heat conduction functional layer is 0.5W/(mK) to 2W/(mK).
The reinforcing material of the cyanate ester/carbon fiber prepreg with high thermal conductivity is one or more of carbon fibers with thermal conductivity of 30W/(m.K) to 200W/(m.K). In a specific embodiment, the reinforcing material may be a carbon fiber having a Japanese Toray company brand of M60JB [ 151.47W/(m.K) ], M55JB [ 155.75W/(m.K) ], M50[ 96.64W/(m.K) ], M46[ 84.29W/(m.K) ], M40JB [ 68.67W/(m.K) ], M35[ 83.93W/(m.K) ], T1000G [ 31.92W/(m.K) ], T800HB [ 35.01W/(m.K) ], Mitsubishi pitch group brand of K63712-12K [ 140W/(m.K) ], K1352U-2K [ 140W/(m.K) ], or the like.
The resin matrix of the cyanate ester/carbon fiber prepreg with high thermal conductivity is cyanate ester resin with uniformly dispersed high thermal conductivity filler. The high thermal conductivity filler is selected from at least one of graphite, aluminum oxide, magnesium oxide, silicon carbide or carbon nano-tubes. In the specific embodiment, the mass of the high-thermal-conductivity functional layer is 100%, the mass content of the high-thermal-conductivity filler is 30% -50%, the filler can be uniformly dispersed and not agglomerated while the surface thermal conductivity of the reinforced material is enhanced, and almost no loss is caused on various performances.
In a preferred embodiment, when the high-thermal-conductivity functional layer adopts the high-thermal-conductivity filler, the high-thermal-conductivity filler is also added into the cyanate ester/carbon fiber composite main body, and the high-thermal-conductivity filler and the cyanate ester/carbon fiber composite main body are matched with each other to achieve double effects, so that the high thermal conductivity of the high-thermal-conductivity cyanate ester-based carbon fiber composite provided by the invention can be better ensured. The mass of the cyanate/carbon fiber composite material main body is 100%, and the mass content of the high-thermal conductivity coefficient filler in the composite material main body is 2% -10%.
The invention also provides a preparation method of the composite material, which comprises the following steps: s1, according to the layering angle and sequence, laying cyanate/carbon fiber prepreg on the mould to obtain a cyanate/carbon fiber composite material main body, and laying a high-heat-conductivity functional layer on the topmost layer of the cyanate/carbon fiber composite material main body; and S2, putting the whole body into a furnace, curing and compression molding to obtain the composite material. Specifically, the high-thermal-conductivity functional layer is obtained by coating cyanate ester resin glue solution of ultrasonically dispersed high-thermal-conductivity filler and then performing hot-melting and pre-dipping with carbon fibers.
The high-thermal conductivity composite material comprises a cyanate/carbon fiber composite material main body and a high-thermal conductivity functional layer, wherein the high-thermal conductivity filler content in the high-thermal conductivity functional layer is high and is consistent with a matrix of the cyanate/carbon fiber composite material main body, so that the interface problem is avoided; the composite material main body can also be obtained by hot-melting and pre-dipping resin films with uniformly dispersed fillers (2-10 wt%) and carbon fibers, and the composite material main body and the fillers with high content in the outer functional layer act together, so that the defects of low filling amount, poor heat conduction effect and influence on other performances in a simple filling method are overcome;
at present, carbon fiber composite materials with high specific strength and high specific rigidity are generally adopted for space optical structures. The heat conductivity of the carbon fiber materials commonly used in China is poor, and the heat conductivity of the carbon fiber materials in the fiber direction is only about 2W/(m.K). The composite material can be used for a space optical structure, can improve the temperature uniformity of a sensor and the like, and the heat conductivity of the truss rods prepared by the composite material is more than 10W/(m.K), so that the steady-state axial temperature difference of the truss rods is less than 2 ℃, and the composite material has important significance for improving the temperature gradient of a low-heat-conductivity structural member on a space optical remote sensor.
In the cyanate ester-based carbon fiber composite material with high thermal conductivity, the high thermal conductivity functional layer is obtained by integrally curing and molding after being combined with the composite material main body by adopting a prepreg laying process, the requirements of complex process and equipment of a coating method are different, interface integrated combination is realized by fewer steps, the process is simple, and industrial production is easy to realize.
The following is a detailed description of specific embodiments.
Example 1
In the cyanate ester-based carbon fiber composite material with high thermal conductivity of the embodiment, the structure of the main body of the cyanate ester/carbon fiber composite material is formed by cyanate ester/carbon fiber prepreg according to [0/90 ]]10The high-thermal-conductivity functional layer is obtained by laying and paving a layer, and the high-thermal-conductivity functional layer is prepared from cyanate ester/carbon fiber prepreg according to the proportion of 02The paving layer is directly paved on the composite material main body; the cyanate/carbon fiber prepreg is prepared by uniformly dispersing high-thermal-conductivity-coefficient filler in cyanate resin in a prepolymerization process by using an ultrasonic instrument, preparing a resin film from the resin system on a coating machine, and performing hot-melt prepreg with M40JB carbon fibers; wherein the high-thermal-conductivity-coefficient filler is graphite, the mass content of the high-thermal-conductivity-coefficient filler in the composite material main body is 5%, and the mass content of the high-thermal-conductivity-coefficient filler in the high-thermal-conductivity functional layer is 50%.
The cyanate/carbon fiber composite material main body and the high-thermal-conductivity functional layer are integrally cured and molded to obtain the final composite material, wherein the thermal conductivity coefficient of the composite material is 11.66W/(m.K), the modulus is 115MPa, and the thermal expansion coefficient is alphaxIs 1.01 x 10-6/K；αyIs 1.51 x 10-6/K。
Example 2
In the cyanate ester-based carbon fiber composite material with high thermal conductivity of the embodiment, the main body of the cyanate ester/carbon fiber composite material is made of cyanate ester carbon fiber prepreg according to [ ± 15 [ ]]8The high-thermal-conductivity functional layer is obtained by laying and paving a layer, and the high-thermal-conductivity functional layer is prepared from cyanate ester/carbon fiber prepreg according to the proportion of 02The paving layer is directly paved on the composite material main body; the cyanate/carbon fiber prepreg is prepared by uniformly dispersing high-thermal-conductivity-coefficient filler in cyanate resin in a prepolymerization process by using an ultrasonic instrument, preparing a resin film from the resin system on a coating machine, and performing hot-melt prepreg with M55JB carbon fibers; wherein the high-thermal conductivity filler is alumina, the mass content of the high-thermal conductivity filler in the composite material main body is 2%, and the high-thermal conductivity in the high-thermal conductivity functional layerThe mass content of the filler is 50%.
The cyanate/carbon fiber composite material main body and the high-thermal-conductivity functional layer are integrally cured and molded to obtain the final composite material, wherein the thermal conductivity coefficient of the composite material is 11.45W/(m.K), the modulus is 213MPa, and the thermal expansion coefficient is alphaxIs-1.83 x 10-6/K；αyIs 17.8 x 10-6The bending strength change rate after ultraviolet irradiation (the absorbed dose is 2000ESH) is-7.9 percent, the bending modulus change rate is 5.7 percent, the interlaminar shear strength change rate is-16.5 percent, and the mass loss rate is-0.25 percent.
Example 3
In the cyanate ester-based carbon fiber composite material with high thermal conductivity of the embodiment, the main body of the cyanate ester/carbon fiber composite material is made of cyanate ester/carbon fiber prepreg according to [0/90/± 45 ]]8The high-thermal-conductivity functional layer is obtained by laying and paving, and is prepared from cyanate ester/carbon fiber prepreg according to the proportion of +/-152The paving layer is directly paved on the composite material main body; the cyanate/carbon fiber prepreg is prepared by uniformly dispersing high-thermal-conductivity-coefficient filler in cyanate resin in a prepolymerization process by using an ultrasonic instrument, preparing a resin film from the resin system on a coating machine, and performing hot-melt prepreg with M55JB carbon fibers; wherein, the high thermal conductivity coefficient filler is alumina and magnesia, the mass content of the high thermal conductivity coefficient filler in the composite material main body is 2 percent, and the mass content of the high thermal conductivity coefficient filler in the high thermal conductivity functional layer is 40 percent.
The cyanate/carbon fiber composite material main body and the high-thermal-conductivity functional layer are integrally cured and molded to obtain the final composite material, wherein the thermal conductivity coefficient of the composite material is 16.95W/(m.K), the modulus is 112MPa, and the thermal expansion coefficient is alphaxIs 0.222 x 10-6/K；αyIs 0.609 x 10-6/K。
Example 4
In the cyanate ester-based carbon fiber composite material with high thermal conductivity of the embodiment, the main body of the cyanate ester/carbon fiber composite material is made of cyanate ester/carbon fiber prepreg according to [0/± 60 ]]10The high-thermal-conductivity functional layer is obtained by laying and paving, and the high-thermal-conductivity functional layer is prepared from cyanate ester/carbon fiber prepreg according to the proportion of +/-302The paving layer is directly paved on the composite material main body;the cyanate/carbon fiber prepreg is prepared by uniformly dispersing high-thermal-conductivity-coefficient fillers in cyanate resin in a prepolymerization process by using an ultrasonic instrument, preparing a resin film from the resin system on a coating machine, and performing hot melt prepreg with M55JB carbon fibers, wherein the high-thermal-conductivity-coefficient fillers are carbon nano tubes, the mass content of the high-thermal-conductivity-coefficient fillers in the composite material main body is 3%, and the mass content of the high-thermal-conductivity-coefficient fillers in the high-thermal-conductivity functional layer is 45%.
The cyanate/carbon fiber composite material main body and the high-thermal-conductivity functional layer are integrally cured and molded to obtain the final composite material, wherein the thermal conductivity coefficient of the composite material is 10.47W/(m.K), the modulus is 106MPa, and the thermal expansion coefficient is alphaxIs 0.253 x 10-6/K；αyIs 0.552 x 10-6K, vacuum conditions (125 ℃, 1 x 10)-3Pa) total mass loss TML is 0.177%, condensable volatile content CVCM 0.005%, water vapor suck-back WVR 0.124%.
Example 5
In the cyanate ester-based carbon fiber composite material with high thermal conductivity of the embodiment, the main body of the cyanate ester/carbon fiber composite material is made of cyanate ester/carbon fiber prepreg according to [0/90/± 45 ]]8The high-thermal-conductivity functional layer is obtained by laying and paving a layer, and the high-thermal-conductivity functional layer is prepared from cyanate ester/carbon fiber prepreg according to the proportion of 02The paving layer is directly paved on the composite material main body; the cyanate/carbon fiber prepreg is prepared by uniformly dispersing high-thermal-conductivity-coefficient filler in cyanate resin in a prepolymerization process by using an ultrasonic instrument, preparing a resin film from the resin system on a coating machine, and performing hot-melt prepreg with T800HB or M55JB carbon fibers; the composite material comprises a composite material main body, a high thermal conductivity functional layer and a high thermal conductivity functional layer, wherein the carbon fiber adopted in the composite material main body is T800HB, and the carbon fiber adopted in the high thermal conductivity functional layer is M55 JB; the high-thermal-conductivity-coefficient filler is silicon carbide, the mass content of the high-thermal-conductivity-coefficient filler in the composite material main body is 10%, and the mass content of the high-thermal-conductivity-coefficient filler in the high-thermal-conductivity functional layer is 50%.
The cyanate/carbon fiber composite material main body and the high-thermal-conductivity functional layer are integrally cured and molded to obtain the final composite material, wherein the thermal conductivity coefficient of the composite material is 10.36W/(m.K), the modulus is 74MPa, and the thermal expansion coefficient is alphaxIs 1.32 x 10-6/K；αyIs 2.23 x 10-6/K。
In conclusion, the cyanate ester-based carbon fiber composite material with high thermal conductivity of the invention is prepared by hot-melting and pre-dipping the resin film with uniformly dispersed fillers and carbon fibers to obtain the composite material main body, and the composite material main body and the fillers with high content of the high thermal conductivity functional layer act together, so that the defects of low filling amount, poor thermal conductivity and influence on other performances in a pure filling method are overcome, and the cyanate ester-based carbon fiber composite material with high thermal conductivity can ensure that other performances are still good while having excellent thermal conductivity.
The cyanate-based carbon fiber composite material with high thermal conductivity can be used for space optical structures, can improve the temperature uniformity of sensors and the like, and the thermal conductivity of truss rods prepared by the cyanate-based carbon fiber composite material is more than 10W/(m.K), so that the steady-state axial temperature difference of the truss rods is less than 2 ℃, and the cyanate-based carbon fiber composite material has important significance for improving the temperature gradient of low thermal conductivity structural parts on space optical remote sensors.
The above-described embodiments of the present invention should not be construed as limiting the scope of the present invention. Any other corresponding changes and modifications made according to the technical idea of the present invention should be included in the protection scope of the claims of the present invention.
Claims (4)
1. The cyanate ester-based carbon fiber composite material with the high thermal conductivity is characterized by comprising a cyanate ester/carbon fiber composite material main body and a high thermal conductivity functional layer, wherein the high thermal conductivity functional layer covers the cyanate ester/carbon fiber composite material main body;
the high-thermal-conductivity functional layer is obtained by laying one or more layers of cyanate ester/carbon fiber prepreg with high thermal conductivity on a cyanate ester/carbon fiber composite material main body according to a certain laying angle;
the reinforcing material of the cyanate ester/carbon fiber prepreg with high thermal conductivity is one or more of carbon fibers with thermal conductivity of 30W/(m.K) -200W/(m.K); the resin matrix is cyanate ester resin with uniformly dispersed high-thermal conductivity filler, and the high-thermal conductivity filler is uniformly dispersed in the cyanate ester resin in the prepolymerization process by using an ultrasonic instrument;
the high-thermal-conductivity-coefficient filler is selected from at least one of graphite, aluminum oxide, magnesium oxide, silicon carbide or carbon nanotubes; the mass of the high-thermal-conductivity functional layer is 100 percent, and the mass of the high-thermal-conductivity coefficient filler is 30-50 percent;
the composite material is obtained by integrally curing and molding the cyanate ester/carbon fiber composite material main body and the high-thermal-conductivity functional layer;
the high-thermal-conductivity-coefficient filler is also added into the main body of the cyanate/carbon fiber composite material, and is uniformly dispersed in cyanate resin in the prepolymerization process by using an ultrasonic instrument, wherein the mass of the main body of the cyanate/carbon fiber composite material is 100%, and the mass content of the high-thermal-conductivity-coefficient filler in the main body of the composite material is 2% -10%.
2. The composite material according to claim 1, wherein the high thermal conductivity functional layer has a thermal conductivity of 0.5W/(m-K) to 2W/(m-K).
3. A method of making the composite material of claim 1, comprising:
s1, according to the layering angle and sequence, laying cyanate/carbon fiber prepreg on a mould to obtain a cyanate/carbon fiber composite material main body, and laying a high-heat-conductivity functional layer on the topmost layer of the cyanate/carbon fiber composite material main body;
and S2, putting the whole body into a furnace, curing and compression molding to obtain the composite material.
4. The preparation method according to claim 3, wherein the high thermal conductive functional layer is prepared by laying a prepreg obtained by coating a cyanate ester resin adhesive solution of an ultrasonically dispersed high thermal conductive filler and then hot-melting and pre-dipping the coated cyanate ester resin adhesive solution with carbon fibers.
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| CN106584965A (en) * | 2016-12-23 | 2017-04-26 | 北京航空航天大学 | High thermal-conductive carbon fiber composite material and preparation method and application thereof |
| CN107323025A (en) * | 2017-08-02 | 2017-11-07 | 北京航空航天大学 | Vertical orientated composite of a kind of interlayer high heat conduction fine hair and preparation method thereof |
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