CN106810719A - A kind of hot functional composite material and its preparation method and application - Google Patents
A kind of hot functional composite material and its preparation method and application Download PDFInfo
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- CN106810719A CN106810719A CN201710104372.2A CN201710104372A CN106810719A CN 106810719 A CN106810719 A CN 106810719A CN 201710104372 A CN201710104372 A CN 201710104372A CN 106810719 A CN106810719 A CN 106810719A
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K9/00—Use of pretreated ingredients
- C08K9/04—Ingredients treated with organic substances
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K3/00—Use of inorganic substances as compounding ingredients
- C08K3/38—Boron-containing compounds
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K5/00—Heat-transfer, heat-exchange or heat-storage materials, e.g. refrigerants; Materials for the production of heat or cold by chemical reactions other than by combustion
- C09K5/02—Materials undergoing a change of physical state when used
- C09K5/06—Materials undergoing a change of physical state when used the change of state being from liquid to solid or vice versa
- C09K5/063—Materials absorbing or liberating heat during crystallisation; Heat storage materials
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K3/00—Use of inorganic substances as compounding ingredients
- C08K3/38—Boron-containing compounds
- C08K2003/382—Boron-containing compounds and nitrogen
- C08K2003/385—Binary compounds of nitrogen with boron
Abstract
The invention provides a kind of hot functional composite material and its preparation method and application, the composite includes phase-change material and orientable heat filling, wherein, relative to the phase-change material of 100 weight portions, orientable heat filling is 0.01 60 weight portions.Above-mentioned composite, when more than phase transition temperature, makes heat filling be orientated perpendicular to direction of heat flow by applying external force, and test obtains the thermal conductivity perpendicular to differently- oriented directivity;Then, change external force direction, filler is set to be orientated parallel to direction of heat flow, it is cooled to below phase transition temperature afterwards, test along the thermal conductivity of differently- oriented directivity, the thermal conductivity reversible mutation multiple of measure can be higher than 5 times, can apply in thermal energy storage, heat energy control (such as hot intelligent switch), building energy conservation, the radiating of microelectronic component, sensing, phonon device, phonon computer field.
Description
Technical field
The present invention relates to hot merit energy field of compound material, and in particular to a kind of thermal conductivity reversible mutation of magnetic tuning it is solid-
Liquid phase change composite material.
Background technology
Heat energy is a kind of abundant energy, and 90% energy production is all flow-related with heat energy in the world, and regrettably
Wherein only 13% can effectively utilize, most of heat energy is consumed in the form of used heat is to Environmental diffusion.How heat energy is improved
Utilization ratio is scientists focus of attention always.Prepared by thermal switch, the typically material by possessing thermal conductivity mutability, i.e.,
The thermal conductivity of material can undergo mutation in a certain temperature, and this change is reversible.At present, the thermal conductivity of pure phase-change material,
2-3 times or so of mutation can occur in solid-liquid phase change, used as temperature adjusting and thermal switch, mutation multiple is too small.There is text
Report is offered, after phase-change material is compound with non-oriented heat filling, thermal conductivity mutation multiple has raising by a small margin, big appointment hair
Raw 4 times or so mutation, but still temperature adjusting, thermal switch, building energy conservation, hot stealthy, radiation detection, quantum letter cannot be met
Use demand of the fields such as breath, heat storage, sensing to thermal conductivity reversible mutation material.
The content of the invention
The present inventor's research finds, when adding orientable heat filling in phase-change material, heat filling orientation can be with
Significantly amplify the effect of thermal conductivity mutation;Wherein, orientable heat filling refers to use (such as magnetic fields) in outer masterpiece
Under orientable heat filling, it is higher than other directions that the orientation refers to its thermal conductivity along differently- oriented directivity.Research finds, can be orientated
Heat filling in outer masterpiece with producing thermal conductivity reversible change (to can be described as being orientated pyrogenicity conductance possibility of reversal under (such as magnetic fields)
Change), meanwhile, phase-change material produces thermal conductivity reversible change (can be described as thermic thermal conductivity reversible change) in temperature change, and
Both thermal conductivity reversible changes can act synergistically, and obtain the bigger composite of thermal conductivity mutation multiple, such that it is able to
Significantly amplify the effect of heat conductivity mutation.Based on this discovery, the present invention is completed.
The first aspect of the invention is to provide a kind of hot functional composite material, the composite include phase-change material and
Orientable heat filling, wherein, relative to the phase-change material of 100 weight portions, orientable heat filling is 0.01-60 weight
Part.
Preferably, relative to the phase-change material of 100 weight portions, orientable heat filling is 0.1-50 weight portions, also excellent
Elect 0.5-30 weight portions as.
Composite of the invention, the orientable heat filling is in the case where outer masterpiece uses (such as magnetic fields) in the phase
When being orientated in change material, there is no substantially reunion.
According to the present invention, the orientable heat filling is selected from orientable heat filling under magnetic fields.The present invention
In, " can be orientated under magnetic fields " refers to that the filler has magnetic responsiveness, i.e., can be orientated under magnetic fields, and the orientation is
Refer to that its thermal conductivity is higher than other directions along differently- oriented directivity.So, can occur can for the thermal conductivity of magnetic tuning for the composite of acquisition
Inverse mutation, the solid-liquid phase change composite that thermal conductivity mutation multiple is dramatically increased.
According to the present invention, the orientable heat filling is selected from orientable heat filling under following magnetic fields
One or more:The intrinsic heat filling with magnetic response, magnetized bar-shaped metal heat-conducting filler, magnetized ceramic are filled out
Material, magnetized sheet heat filling and magnetized tubulose heat filling.The intrinsic heat filling with magnetic response is selected from this
Levy the ferriferrous oxide particles with magnetic response, the oxide particle of cobalt, oxide particle of nickel etc..The magnetized bar-shaped gold
Category heat filling is selected from magnetized copper nano-wire, magnetized nanowires of gold, magnetized nano silver wire etc..The magnetized ceramics are led
Hot filler is selected from magnetized alumina whisker, magnetized silicon carbide whisker etc..The magnetized sheet heat filling is selected from magnetization
Micron and/or nm-class boron nitride, magnetized Graphene, magnetized graphite etc..The magnetized tubulose heat filling is selected from magnetic
The SWCN of change, magnetized double-walled carbon nano-tube, magnetized multi-walled carbon nano-tubes etc..
Preferably for magnetized bar-shaped metal heat-conducting filler, its draw ratio is 2-1000;For magnetized sheet heat conduction
Filler, its is a diameter of 1-50 microns, and thickness is 0.2-100 nanometers;For magnetized tubulose heat filling (such as magnetized single wall carbon
Nanotube, magnetized double-walled carbon nano-tube, magnetized multi-walled carbon nano-tubes etc.), its draw ratio is:2-1000.
According to the present invention, the phase-change material is selected from one or more of following phase-change materials:Alkane derivative or its
Mixture, organic acid compound, alcohol compound, diamine compounds, ester type compound.Preferably, the alkanes
Compound or its mixture are selected from higher aliphatic hydrocarbon or its mixture.Preferably, the alcohol compound is selected from polyethylene glycol.It is preferred that
Ground, the diamine compounds are selected from butanediamine;The ester type compound is selected from butyl stearate;The higher aliphatic hydrocarbon mixing
Thing is selected from paraffin (preferred, fusing point is 20-60 DEG C of paraffin);The molecular weight of the polyethylene glycol be 500-20000 (preferably
2000-10000, also preferably 3000-6000).
According to the present invention, the hot functional composite material is heat regulation and control composite, and specially one kind is under magnetic fields
The solid-liquid phase change composite of thermal conductivity reversible mutation.
The second aspect of the invention is to provide a kind of preparation method of above-mentioned hot functional composite material, and methods described includes
Following steps:The solid phase change material of 100 weight portions is heated to liquid condition, phase transformation of the control temperature in the phase-change material
More than temperature, the orientable heat filling of the lower addition 0.01-60 weight portions of stirring is continuously stirring to after being well mixed, and is obtained
The composite.
The third aspect of the invention is to provide a kind of method that thermal conductivity for improving phase-change material is mutated multiple, and it includes
Following steps:
S1. orientable heat filling is added in the phase-change material, wherein, relative to the phase transformation material of 100 weight portions
Material, the addition of orientable heat filling is 0.01-60 weight portions.
Methods described is further comprising the steps:
S2. the phase-change material that orientable heat filling will be with the addition of is placed in external force effect (such as magnetic field), in outer masterpiece
With under (such as magnetic fields), orientable heat filling realizes orientation, causes thermal conductivity to be mutated the raising of multiple.
Step S1 also includes:After adding orientable heat filling, ultrasonic agitation 1-60 minutes, the heat filling is obtained
The dispersed composite in phase-change material.
Step S2 is specifically included:The composite that step S1 is obtained is heated to more than phase transition temperature, at such a temperature, will
Composite is placed in external force effect (such as magnetic field), and in outer masterpiece with (such as magnetic fields), orientable heat filling is realized
Perpendicular to direction of heat flow orientation, determine along the thermal conductivity in vertical orientated direction;Then, external force effect (such as magnetic field) direction is changed,
Make heat filling realize being orientated along parallel to direction of heat flow, be cooled to below phase transition temperature afterwards, survey along the thermal conductivity of differently- oriented directivity
Rate;Two ratios of thermal conductivity (high level/low value) are the thermal conductivity mutation multiple of the composite.
Preferably, the magnetic field intensity in the magnetic field is not in 0-1000mT and including 0, it is preferable that magnetic field intensity is between 10-
Between 500mT, it is further preferred that between 20-300mT.
The fourth aspect of the invention is to provide a kind of powe control, and it uses above-mentioned hot functional composite material.
The powe control is, for example, hot intelligent switch.
The fifth aspect of the invention is to provide a kind of application of above-mentioned hot functional composite material, the hot merit energy composite wood
Material can be applied to thermal energy storage, heat energy control (such as hot intelligent switch), building energy conservation, the radiating of microelectronic component, sensing, sound
The fields such as sub- device, phonon computer.
Beneficial effects of the present invention:
The present invention provides a kind of hot functional composite material, and the composite has the effect of the thermal conductivity mutation for significantly improving
Really (its thermal conductivity mutation multiple is higher than 5, it might even be possible to higher than 10), (such as hot intelligent switch) when being controlled for heat energy, temperature
Degree ability of regulation and control is stronger, and the speed of regulation and control is faster;Possesses the composite of the performance in thermal energy storage, building energy conservation, micro-
The fields such as radiating, sensing, phonon device, the phonon computer of electronic device also possess application value.
Specific embodiment
In one embodiment of the invention, the orientable heat filling is led selected from orientable under magnetic fields
Hot filler, can be prepared using following methods:The heat filling of non-oriented is dispersed in water, polystyrolsulfon acid is subsequently adding
Sodium, by the regulation of acidity, control kayexalate absorption is on the heat filling of the non-oriented;It is scrubbed, dry
Afterwards, the heat filling that will be adsorbed with kayexalate is dispersed in water again again, adds frerrous chloride and ferric trichloride, stirring
Lower addition 1,6- hexamethylene diamines, obtain dark brown suspension, after scrubbed, drying, obtain to be orientated under magnetic fields of the invention
Heat filling.
The heat filling of the non-oriented is selected from bar-shaped metal heat-conducting filler, ceramic filler, sheet heat conduction and fills out
Material and tubulose heat filling.The bar-shaped metal heat-conducting filler is selected from copper nano-wire, nanowires of gold, nano silver wire etc..The pottery
Porcelain heat filling is selected from alumina whisker, silicon carbide whisker etc..The sheet heat filling is selected from micron and nm-class boron nitride, stone
Black alkene, graphite etc..The tubular filler is selected from SWCN, double-walled carbon nano-tube, multi-walled carbon nano-tubes etc..
With reference to specific embodiment, the present invention is expanded on further.It should be understood that these embodiments are merely to illustrate the present invention
Rather than limitation the scope of the present invention.Furthermore, it is to be understood that after described content of the invention has been read, this area skill
Art personnel can make various changes or modifications to the present invention, and these equivalent form of values equally fall within limited range of the present invention.
Comparative example 1:
Macrogol 4000 (PEG4000) phase-change material, Measured Results of Thermal Conductivity is as follows:
(1) by PEG4000 heating for dissolving (temperature is T1), its thermal conductivity factor under temperature T1 is tested in a liquid state
Size;
(2) PEG4000 is cooled to below phase transition temperature (temperature is T2), is tested under temperature T2 under its solid state
Thermal conductivity factor size;
The ratio (high level/low value) of above-mentioned two thermal conductivity factor is the thermal conductivity mutation multiple of the phase-change material, test
The results are shown in Table 1.
Comparative example 2:
By the unmagnetized boron nitride filler (i.e. the heat filling of non-oriented) of 5 weight portions, 5 microns of diameter, thickness 100 is received
Rice, is added in the PEG4000 of 100 weight portions dissolving, the lower stirring of insulation 1 hour, at said temperatures under test liquid state
Thermal conductivity factor size;Solution is cooled to below phase transition temperature (temperature is T2), is tested under temperature T2 under its solid state
Thermal conductivity factor size;The ratio (high level/low value) of above-mentioned two thermal conductivity factor is the thermal conductivity mutation times of the phase-change material
Number, test result is listed in Table 1 below.
Embodiment 1
(1) by a diameter of 5 microns of 100g, the boron nitride that thickness is 100 nanometers, it is distributed in 1L water, is subsequently adding
1mol/L kayexalates, add the hydrochloric acid of 1mol/L, regulation pH value to 4.0 or so, it is ensured that kayexalate is complete
Adsorb on boron nitride entirely.Then diafiltration three times are crossed with water and acetic acid, is dried afterwards, the nitrogen of kayexalate will be adsorbed with
Change boron to be scattered in deionized water again, add frerrous chloride and ferric trichloride, stirring is lower to add 1,6- hexamethylene diamines, dark until obtaining
Brown suspension, washes amine molecule with water, and 70 DEG C of drying obtain orientable conductive particle (i.e. magnetized nitrogen under magnetic fields
Change boron).
(2) the solid PEG4000 of 100 weight portions is heated to liquid condition, control temperature is in its phase in being put in water-bath
More than temperature stir, the magnetized boron nitride that (1) obtains the step of 5 weight portion is added during stirring, connect under ultrasound
Continuous stirring is placed under 20mT magnetic fields to after being well mixed, and magnetized boron nitride is realized, perpendicular to direction of heat flow orientation, determining edge
The thermal conductivity in vertical orientated direction;Then, change magnetic direction, magnetized boron nitride is realized that edge takes parallel to direction of heat flow
To, it is cooled to below phase transition temperature afterwards, survey along the thermal conductivity of differently- oriented directivity;Two ratios of thermal conductivity (high level/low value) are
The thermal conductivity mutation multiple of the composite, test result is listed in Table 1 below.
Embodiment 2
Other are only that magnetic field intensity is adjusted to 60mT by 20mT with embodiment 1.
Embodiment 3
Other are only that boron nitride is changed into Graphene with embodiment 2.
Embodiment 4-6
Other are only boron nitride to be changed to multi-walled carbon nano-tubes respectively (draw ratio is 50, nanowires of gold (long with embodiment 2
Footpath ratio for 100), silicon carbide whisker.
Table 1
In table 1, it is described as follows at *:In comparative example 1 and 2, the data of first row (are led for the thermal conductivity under solid state
Hot coefficient), the data of secondary series are the thermal conductivity (i.e. thermal conductivity factor) under liquid condition, unrelated with differently- oriented directivity.
More than, embodiments of the present invention are illustrated.But, the present invention is not limited to above-mentioned implementation method.It is all
Within the spirit and principles in the present invention, any modification, equivalent substitution and improvements done etc., should be included in guarantor of the invention
Within the scope of shield.
More than, embodiments of the present invention are illustrated.But, the present invention is not limited to above-mentioned implementation method.It is all this
Within the spirit and principle of invention, any modification, equivalent substitution and improvements done etc. should be included in protection model of the invention
Within enclosing.
Claims (10)
1. a kind of hot functional composite material, it is characterised in that the composite includes that phase-change material and orientable heat conduction are filled out
Material, wherein, relative to the phase-change material of 100 weight portions, orientable heat filling is 0.01-60 weight portions.
Preferably, relative to the phase-change material of 100 weight portions, orientable heat filling is 0.1-50 weight portions, also preferably
0.5-30 weight portions.
2. hot functional composite material according to claim 1, it is characterised in that the orientable heat filling is selected from down
One or more of orientable heat filling under the magnetic fields stated:The intrinsic heat filling with magnetic response, magnetized rod
Shape metal heat-conducting filler, magnetized ceramic filler, magnetized sheet heat filling and magnetized tubulose heat filling.
Preferably, the intrinsic heat filling with magnetic response is selected from the intrinsic ferriferrous oxide particles with magnetic response, cobalt
Oxide particle, the oxide particle of nickel etc..
Preferably, the magnetized bar-shaped metal heat-conducting filler is selected from magnetized copper nano-wire, magnetized nanowires of gold, magnetized
Nano silver wire etc..
Preferably, the magnetized ceramic filler is selected from magnetized alumina whisker, magnetized silicon carbide whisker etc..
Preferably, the magnetized sheet heat filling be selected from magnetized micron and/or nm-class boron nitride, magnetized Graphene,
Magnetized graphite etc..
Preferably, the magnetized tubulose heat filling is selected from magnetized SWCN, magnetized double-walled carbon nano-tube, magnetic
Multi-walled carbon nano-tubes of change etc..
3. hot functional composite material according to claim 2, it is characterised in that filled out for magnetized bar-shaped metal heat-conducting
Material, its draw ratio is 2-1000;For magnetized sheet heat filling, its is a diameter of 1-50 microns, and thickness is received for 0.2-100
Rice;For magnetized tubulose heat filling (such as magnetized SWCN, magnetized double-walled carbon nano-tube, magnetized many walls
CNT etc.), its draw ratio is:2-1000.
4. the hot functional composite material according to claim any one of 1-3, it is characterised in that the phase-change material is selected from down
State phase-change material one or more:Alkane derivative or its mixture, organic acid compound, alcohol compound, diamines
Class compound, ester type compound.
Preferably, the alkane derivative or its mixture are selected from higher aliphatic hydrocarbon or its mixture.
Preferably, the alcohol compound is selected from polyethylene glycol.
Preferably, the diamine compounds are selected from butanediamine;
Preferably, the ester type compound is selected from butyl stearate;
Preferably, the higher aliphatic hydrocarbon mixture is selected from paraffin (preferred, fusing point is 20-60 DEG C of paraffin);
Preferably, the molecular weight of the polyethylene glycol is 500-20000 (preferably 2000-10000, also preferably 3000-
6000)。
5. the preparation method of the hot functional composite material described in any one of claim 1-4, it is characterised in that methods described includes
Following steps:The solid phase change material of 100 weight portions is heated to liquid condition, phase transformation of the control temperature in the phase-change material
More than temperature, the orientable heat filling of the lower addition 0.01-60 weight portions of stirring is continuously stirring to after being well mixed, and is obtained
The composite.
6. a kind of method that thermal conductivity for improving phase-change material is mutated multiple, it is characterised in that the described method comprises the following steps:
S1. orientable heat filling is added in the phase-change material, wherein, relative to the phase-change material of 100 weight portions, can
The addition of the heat filling of orientation is 0.01-60 weight portions.
Preferably, methods described is further comprising the steps:
S2. the phase-change material that orientable heat filling will be with the addition of is placed in external force effect (such as magnetic field), in outer masterpiece with (such as
Magnetic fields) under, orientable heat filling realizes orientation, causes thermal conductivity to be mutated the raising of multiple.
7. method according to claim 6, it is characterised in that step S1 also includes:After adding orientable heat filling,
Ultrasonic agitation 1-60 minutes, obtain the dispersed composite in phase-change material of the heat filling.
8. method according to claim 7, it is characterised in that step S2 is specifically included:The composite wood that step S1 is obtained
Material is heated to more than phase transition temperature, at such a temperature, composite is placed in external force effect (such as magnetic field), is used in outer masterpiece
Under (such as magnetic fields), orientable heat filling is realized, perpendicular to direction of heat flow orientation, determining along the heat in vertical orientated direction
Conductance;Then, change external force effect (such as magnetic field) direction, make heat filling realize being orientated along parallel to direction of heat flow, drop afterwards
Below temperature to phase transition temperature, survey along the thermal conductivity of differently- oriented directivity;Two ratios of thermal conductivity (high level/low value) are the composite wood
The thermal conductivity mutation multiple of material.
Preferably, the magnetic field intensity in the magnetic field is not in 0-1000mT and including 0;Preferably, magnetic field intensity is between 10-500mT
Between;It is further preferred that between 20-300mT.
9. a kind of powe control, it is characterised in that described device can be answered using the hot merit described in claim any one of 1-4
Condensation material.
Preferably, the powe control is, for example, hot intelligent switch.
10. the application of the hot functional composite material described in any one of claim 1-4, it is characterised in that the hot function and service
Materials application is in thermal energy storage, heat energy control (such as hot intelligent switch), building energy conservation, the radiating of microelectronic component, sensing, sound
The fields such as sub- device, phonon computer.
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