AU2020102327A4 - Anisotropic Thermally Conductive Multilayer Polymer Composite Material and Preparation Method Thereof - Google Patents
Anisotropic Thermally Conductive Multilayer Polymer Composite Material and Preparation Method Thereof Download PDFInfo
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- H01B1/00—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors
- H01B1/06—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors mainly consisting of other non-metallic substances
- H01B1/12—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors mainly consisting of other non-metallic substances organic substances
- H01B1/124—Intrinsically conductive polymers
- H01B1/128—Intrinsically conductive polymers comprising six-membered aromatic rings in the main chain, e.g. polyanilines, polyphenylenes
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- B32B27/00—Layered products comprising a layer of synthetic resin
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- B32B27/00—Layered products comprising a layer of synthetic resin
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- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/40—Layered products comprising a layer of synthetic resin comprising polyurethanes
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- B32B37/00—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding
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- B32B9/005—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00 comprising one layer of ceramic material, e.g. porcelain, ceramic tile
- B32B9/007—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00 comprising one layer of ceramic material, e.g. porcelain, ceramic tile comprising carbon, e.g. graphite, composite carbon
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
- H01B1/00—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors
- H01B1/20—Conductive material dispersed in non-conductive organic material
- H01B1/24—Conductive material dispersed in non-conductive organic material the conductive material comprising carbon-silicon compounds, carbon or silicon
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B32B2264/00—Composition or properties of particles which form a particulate layer or are present as additives
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- B32B2307/00—Properties of the layers or laminate
- B32B2307/30—Properties of the layers or laminate having particular thermal properties
- B32B2307/302—Conductive
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- B32—LAYERED PRODUCTS
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- B32B2313/00—Elements other than metals
- B32B2313/02—Boron
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Abstract
The present invention relates to the technical field of composite materials, and provides an
anisotropic thermally conductive multilayer polymer composite material and a preparation
method thereof. The present invention makes use of interfacial tension at an interface of an
immiscible two-layer system which has a dispersing effect on a thermally conductive filler, so
that the thermally conductive filler can be uniformly dispersed at an intermediate interface of
the immiscible two-layer system. When a polymer film passes through the intermediate
interface of the immiscible two-layer system, the thermally conductive filler pushed by the bar
can be oriented and continuously arranged on a surface of the polymer film, forming an
oriented thermally conductive network on and parallel to the surface of the polymer film. At
the same time, since the thermally conductive filler forms a thermally conductive network
parallel to and on the surface of the polymer film, heat transfer is faster in a stacking direction
of the multilayer polymer composite material than in a normal line direction of the stacking.
That is, the obtained anisotropic thermally conductive multilayer polymer composite material
has a higher thermal conductivity coefficient in the in-plane direction than in the normal
direction, showing anisotropic thermal conductivity.
14
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2 3
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FIG. 1
Normal direction
FIG. 2
Description
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2 3
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FIG. 1
Normal direction
FIG. 2
ANISOTROPIC THERMALLY CONDUCTIVE MULTILAYER POLYMER COMPOSITE MATERIAL AND PREPARATION METHOD THEREOF TECHNICAL FIELD The present invention relates to the technical field of composite materials, and in particular to an anisotropic thermally conductive multilayer polymer composite material and a preparation method thereof. BACKGROUND Thermal failure is one of the most important failure modes in electronic packaging. According to statistics, when an operating temperature of a device rises by 10°C, reliability of the device drops by 50%. Therefore, in such fields as such as aerospace and military, electronic equipment, power electronic equipment, optoelectronic devices, micro/nano electromechanical systems, solid-state lighting and solar cells all require heat dissipation and cooling. Traditional thermal conductive materials such as metals, metal oxides and nitride ceramics have excellent thermal conductivity, but they have their own limitations such as a heavy weight, which can no longer meet the requirements in development of modern electronic technology. Addition of inorganic fillers with functional features to polymers by a physical or chemical method can effectively combine advantages of the polymer such as lightness, easy processing and corrosion resistance with functionality of inorganic substances. Use of particles with excellent thermal conductivity (for example, metals, carbons and ceramics) as thermally conductive fillers in preparation of thermally conductive composite materials is expected to meet the requirements of thermally conductive materials in motor electrical, electronic packaging, aerospace and military fields and other fields. However, conductivity of a polymer matrix composite material is not only related to properties of the filler itself (for example, material structure, thermal conductivity, electrical conductivity, size and morphology), but also closely related to dispersion state and structural order of the filler in the polymer matrix. The patent document CN105733065A entitled "Anisotropic Thermally Conductive Polymer Composite Material and Preparation Method Thereof' discloses a method for preparing a thermally conductive polymer composite material by a melt blending method combined with a magnetic field to induce orientation and arrangement of thermally conductive particles. However, highly thermally conductive ceramic powders in polymer matrix of a polymer matrix composite material oriented and arranged by a magnetic field can hardly form a thermally conductive network, and there is still a serious interface thermal resistance between fillers and resins.
SUMMARY In view of this, an objective of the present invention is to provide an anisotropic thermally conductive multilayer polymer composite material and a preparation method thereof. With this method, an oriented thermally conductive network of thermally conductive fillers can be formed on a surface of the polymer, thereby improving thermal conductivity of the polymer composite material. In order to realize the objective of the present invention, the present invention provides the following technical solutions: The present invention provides a method for preparing an anisotropic thermally conductive multilayer polymer composite material, including the following steps: step (1): providing a thermally conductive filler dispersion; step (2): adding the thermally conductive filler dispersion to an immiscible two-layer system which includes an upper layer system as a liquid phase or a gas phase and a lower layer system as a liquid phase, where a thermally conductive filler is oriented and dispersed at an intermediate interface of the immiscible two-layer system; step (3): immersing a polymer film in the lower layer system of the immiscible two-layer system containing the thermally conductive filler, moving the polymer film obliquely upward and at the same time pushing the thermally conductive filler horizontally towards the polymer film at a constant speed by using a bar having a width greater than or equal to that of the polymer film, so that the thermally conductive filler is attached to a surface of the polymer film; and removing the polymer film attached with the thermally conductive filler completely from the immiscible two-layer system to obtain a thermally conductivefiller/polymer composite film; step (4): stacking or winding the thermally conductive filler/polymer composite film, and subjecting to heat treatment to obtain an anisotropic thermally conductive multilayer polymer composite material. Preferably, the thermally conductive filler is one or more of boron nitride, graphite, graphene, carbon nanotube and carbon fiber; a particle size of the thermally conductive filler is 0.01-100 [m; a dispersant of the thermally conductive filler dispersion is one or more of ethanol, isopropanol, N,N'-dimethylformamide and N-methylpyrrolidone; and a mass concentration of the thermally conductive filler in the thermally conductive filler dispersion is 0.1-10%. Preferably, the immiscible two-layer system includes one of n-hexane-water system, cyclohexane-water system, octane-water system, air-water system, acetone-water system and water-carbon tetrachloride system; and a volume ratio of the thermally conductive filler dispersion to the lower layer system of the immiscible two-layer system is (0.001-1):1. Preferably, a material of the polymer film is one or more of polypropylene, polyethylene, polystyrene, polycarbonate, acrylonitrile styrene butadiene copolymer, polyamide, polyethylene terephthalate, polyphenylene ether, polyphenylene sulfide, rigid polyvinyl chloride, polymethyl methacrylate, polyformaldehyde, polysulfone, polyimide, polytetrafluoroethylene, polytrifluorochloroethylene, polyperfluoroethylene propylene, polybutylene terephthalate, chlorinated polyether, styrene butadiene rubber, nitrile rubber, silicone rubber, butadiene rubber, polyisoprene, ethylene propylene rubber and neoprene; and a thickness of the polymer film is 1 m- 1 cm. Preferably, an angle between a direction of moving the polymer film obliquely upward and a horizontal direction is 1-90°; a speed of moving the polymer film obliquely upward is 0.001-1 m/s; and a force applied to the bar when pushing the thermally conductive filler is 0.0001-10 N. Preferably, a volume percentage of the thermally conductive filler in the thermally conductive filler/polymer composite film is 0.01-90%. Preferably, the stacking is carried out with 2-200 layers; or the winding is carried out for 2-200 turns. Preferably, the heat treatment is carried out at 30-150°C for 2-24 h. The present invention provides an anisotropic thermally conductive multilayer polymer composite material prepared by the above preparation method. The composite material includes sequentially stacked multiple layers of thermally conductive filler/polymer composite films. The thermally conductive filler/polymer composite films include a polymer film and a thermally conductive filler which forms an oriented thermally conductive network on a surface of the polymer film. The present invention provides a method for preparing an anisotropic thermally conductive multilayer polymer composite material. The method makes use of the interfacial tension at the interface of the immiscible two-layer system which has a dispersing effect on the thermally conductive filler, so that the thermally conductive filler can be uniformly dispersed at the intermediate interface of the immiscible two-layer system. When the polymer film passes through the intermediate interface of the immiscible two-layer system, the thermally conductive filler pushed by a bar can be oriented and continuously arranged on the surface of the polymer film, forming an oriented thermally conductive network on and parallel to the surface of the polymer film. At the same time, since the thermally conductive filler is oriented and continuously arranged on the surface of the polymer film, a contact area between the thermally conductive filler and the polymer film is increased. The increased contact area can reduce the interfacial thermal resistance between the thermally conductive filler and the polymer film and thereby increase thermal conductivity of the composite material. In the present invention, there is no need to modify the surface of the thermally conductive filler, and no defect is introduced to the surface of the thermally conductive filler which is responsible for decrease of intrinsic thermal conductivity of the composite material. At the same time, since the thermally conductive filler forms a thermally conductive network parallel to and on the surface of the polymer film, heat transfer is faster in a stacking direction of the multilayer polymer composite material (i.e. in-plane direction) than in a normal line direction of the stacking (i.e. normal direction). That is, the obtained anisotropic thermally conductive multilayer polymer composite material has a higher thermal conductivity coefficient in the in-plane direction than in the normal direction, showing anisotropic thermal conductivity. Results of examples show that, the anisotropic thermally conductive multilayer polymer composite material obtained by the method of the present invention has an in-plane thermal conductivity coefficient of 9.13 W/m-K and a normal thermal conductivity coefficient of 0.146 W/m-K. At the same time, the method provided by the present invention has simple operations and thus is easy for industrialized mass production. BRIEF DESCRIPTION OF DRAWINGS By way of example only, preferred embodiments of the present invention are described in detail, with reference to the accompanying drawings in which: FIG. 1 schematically shows the thermally conductive filler pushed by the bar; FIG. 2 schematically shows a structure of the anisotropic thermally conductive multilayer polymer composite material; FIG. 3 shows a scanning electron microscopic (SEM) image of the anisotropic thermally conductive multilayer polymer composite material obtained in Example 1 in an in-plain direction; and FIG. 4 shows an SEM image of a cross section of the anisotropic thermally conductive multilayer polymer composite material obtained in Example 1; where in FIGs. 1-2, 1 is a bar, 2 is a thermally conductive filler, 3 is a polymer film, 4 is an intermediate interface of an immiscible two-layer system, 5 is a polymer flm and 6 is a thermally conductive filler. DETAILED DESCRIPTION The present invention provides a method for preparing an anisotropic thermally conductive multilayer polymer composite material, including the following steps: step (1): providing a thermally conductive filler dispersion; step (2): adding the thermally conductive filler dispersion to an immiscible two-layer system which includes an upper layer system as a liquid phase or a gas phase and a lower layer system as a liquid phase, where a thermally conductive filler is oriented and dispersed at an intermediate interface of the immiscible two-layer system; step (3): immersing a polymer film in the lower layer system of the immiscible two-layer system containing the thermally conductive filler, moving the polymer film obliquely upward and at the same time pushing the thermally conductive filler horizontally towards the polymer film at a constant speed by using a bar having a width greater than or equal to that of the polymer film, so that the thermally conductive filler is attached to a surface of the polymer film; and removing the polymer film attached with the thermally conductive filler completely from the immiscible two-layer system to obtain a thermally conductivefiller/polymer composite film; step (4): stacking or winding the thermally conductive filler/polymer composite film, and subjecting to heat treatment to obtain an anisotropic thermally conductive multilayer polymer composite material. The present invention provides a thermally conductive filler dispersion at first. In the present invention, a method of preparing the thermally conductive filler dispersion preferably includes: mixing a thermally conductive filler and a dispersant, and ultrasonicating to obtain a thermally conductive filler dispersion. In the present invention, the thermally conductive filler is preferably one or more of boron nitride, graphite, graphene, carbon nanotube and carbon fiber. In the present invention, the boron nitride is preferably a boron nitride nanosheet, the graphite is preferably a graphite nanosheet. In the present invention, the thermally conductive filler preferably has a particle size of 0.01-100 mi, more preferably 1-50 m. In the present invention, the dispersant is preferably one or more of ethanol, isopropanol, N,N'-dimethylformamide and N-methylpyrrolidone. In the present invention, the ultrasonicating is carried out at a power of preferably
100-1,000 W and more preferably 300-500 W for preferably 1-12 h and more preferably 4-8 h. In the present invention, a mass concentration of the thermally conductive filler in the thermally conductive filler dispersion is preferably 0.1-10%, and more preferably 1-5%. In the present invention, the immiscible two-layer system preferably includes one of n-hexane-water system, cyclohexane-water system, octane-water system, air-water system, acetone-water system and water-carbon tetrachloride system. The present invention has no special requirements on a volume ratio of the upper layer system to the lower layer system, as long as a stable intermediate interface can be formed. In the present invention, a volume ratio of the thermally conductive filler dispersion to the lower layer system of the immiscible two-layer system is preferably (0.001-1):1 and more preferably (0.01-0.5):1. In the present invention, after the thermally conductive filler dispersion is added to the immiscible two-layer system, an interfacial tension in the immiscible two-layer system changes, so that the thermally conductive filler is gathered at the intermediate interface from the dispersion. After the thermally conductive filler is dispersed at the intermediate interface of the immiscible two-layer system, it is preferred in the present invention that, a bar is used to confine the thermally conductive filler in a certain region to increase the distribution density of the thermally conductive filler. In the present invention, a material of the polymer film is preferably one or more of polypropylene, polyethylene, polystyrene, polycarbonate, acrylonitrile styrene butadiene copolymer, polyamide, polyethylene terephthalate, polyphenylene ether, polyphenylene sulfide, rigid polyvinyl chloride, polymethyl methacrylate, polyformaldehyde, polysulfone, polyimide, polytetrafluoroethylene, polytrifluorochloroethylene, polyperfluoroethylene propylene, polybutylene terephthalate, chlorinated polyether, styrene butadiene rubber, nitrile rubber, silicone rubber, butadiene rubber, polyisoprene, ethylene propylene rubber and neoprene. The polymer film preferably has a thickness of 1 m- 1 cm, and more preferably 150-500 [m. The present invention has no special requirements on length and width of the polymer film, and a corresponding design can be made according to actual conditions. In the present invention, an angle between a direction of moving the polymer film obliquely upward and a horizontal direction is preferably 1-90°, and more preferably 30-60°. The polymer film is moved obliquely upward at a speed of preferably 0.001-1 m/s, and more preferably 0.1-0.5 m/s. In the present invention, the thermally conductive filler pushed by the bar is schematically shown in FIG. 1. In the present invention, a material of the bar is preferably polytetrafluoroethylene and/or stainless steel. In the present invention, the bar has a width greater than or equal to that of the polymer film. In the present invention, a force applied to the bar when pushing the thermally conductive filler is preferably 0.0001-10 N, and more preferably 0.01-5 N. The bar is moved at a speed of preferably 0.001-1 m/s, and more preferably 0.1-0.5 m/s. The present invention has no special requirements on the way of applying the force, and a corresponding force applied by a device well known to a person skilled in the art is sufficient, for example, a program-controlled stepping motor or an LB film analyzer. In the present invention, pushing with the bar is carried out, so that the thermal conductive filler is oriented and continuously arranged on the surface of the polymer film and forms a thermally conductive network on and parallel to the surface of the polymer film. After the polymer film attached with the thermally conductive filler is completely removed from the immiscible two-layer system, a thermally conductive filler/polymer composite film is obtained. In the present invention, a volume percentage of the thermally conductive filler in the thermally conductive filler/polymer composite film is preferably 0.01-90%, and more preferably 1-50%. The present invention preferably further includes drying the obtained thermally conductive filler/polymer composite film at preferably 25-100°C and more preferably 40-65°C for preferably 10-60 min and more preferably 20-40 min. In the present invention, stacking or winding the thermally conductivefiller/polymer composite film is carried out followed by subjection to heat treatment to obtain an anisotropic thermally conductive multilayer polymer composite material. In the present invention, before the stacking, the thermally conductive filler/polymer composite flm is preferably cut into a same size. In the present invention, the stacking is carried out with preferably 2-200 layers and more preferably 50-100 layers. The present invention has no special requirements on the way of stacking, and either manual stacking or mechanical stacking can be carried out. In the present invention, after the stacking, a polymer film without a thermally conductive filler is preferably applied on the surface of the outermost thermally conductive filler. In the present invention, the winding is carried out for preferably 2-200 turns, and more preferably 50-100 turns. The present invention has no special requirement on the way of winding, and either manual winding or mechanical winding can be carried out. During the winding, the polymer film of the thermally conductive filler/polymer composite film is positioned on an outer side. In the present invention, after the heat treatment, the anisotropic thermally conductive multilayer polymer composite material is cut. The present invention has no special requirements on the cutting shape as long as the shape can meet actual use requirements. The present invention has no special requirements on the cutting manner, and a cutting manner well known to a person skilled in the art can be used, for example, specifically a rotary shearing machine or a rotary razor cutting tool can be used. In the present invention, the heat treatment is carried out at preferably 30-150°C and more preferably 80-100°C for preferably 2-24 h and more preferably 12 h. In the present invention, the heat treatment is carried out so that the stacked or wound polymer film and thermally conductive filler can bind to each other to form an anisotropic thermally conductive multilayer polymer composite material piece. The present invention provides an anisotropic thermally conductive multilayer polymer composite material prepared by the above preparation method. In the present invention, the anisotropic thermally conductive multilayer polymer composite material includes sequentially stacked multiple layers of thermally conductive filler/polymer composite films. The thermally conductive filler/polymer composite films include a polymer film and a thermally conductive filler which forms an oriented thermally conductive network on a surface of the polymer film. In the present invention, the stacking of the thermally conductive filler/polymer composite film is carried out with preferably 2-200 layers, more preferably 50-100 layers. As a specific embodiment of the present invention, a structure of the anisotropic thermally conductive multilayer polymer composite material is schematically shown in FIG. 2. In the present invention, the anisotropic thermally conductive multilayer polymer composite material has an in-plane thermal conductivity coefficient higher than a normal thermal conductivity coefficient. The anisotropic thermally conductive multilayer polymer composite material and the preparation method thereof provided by the present invention are described below in detail in combination with examples. However, the following description cannot be understood as a limit to the protection scope of the present invention. Example 1 (1) 1 g of boron nitride (with a particle size of 10-18 m) was added to 100 g of ethanol, and ultrasonicated at 100 W for 2 h to obtain a1 wt.% boron nitride dispersion. (2) 10 mL of the boron nitride dispersion was added to 1,000 mL of water. After the boron nitride was evenly dispersed on the water surface, a silicone rubber film with a length of 50 cm, a width of 30 cm and a thickness of 0.2 mm was positioned below the water surface obliquely at an angle of 30 with respect to the horizontal direction. The silicon rubber was moved upwards in the oblique direction at a speed of 5 mm/s. At the same time, a stainless steel bar with a width of 35 cm was applied with a force of 2 N to push the boron nitride horizontally towards the silicon rubber film at a constant speed, so that the boron nitride was attached to the surface of the silicone rubber film. (3) The silicone rubber film was completely removed from the water and dried at 60°C for min to obtain a boron nitride/silicone rubber composite film. (4) The boron nitride/silicone rubber composite film was cut into strips with a width of 5 mm, manually stacked to achieve 200 layers, and then heat treated in an oven at 100°C for 12 h to obtain an anisotropic thermally conductive multilayer polymer composite material. After tests according to "ASTM E 1530-19", the obtained composite material was determined to have an in-plane thermal conductivity coefficient of 0.325 W/m-K and a normal thermal conductivity coefficient of 0.136 W/m-K. An SEM image of obtained anisotropic thermally conductive multilayer polymer composite material in an in-plain direction was shown in FIG. 3. It can be seen from FIG. 3 that, boron nitride thermally conductive fillers were distributed in an oriented direction on a surface of the silicone rubber film. An SEM image of a cross section of the obtained anisotropic thermally conductive multilayer polymer composite material was shown in FIG. 4. It can be seen from FIG. 4 that, boron nitride thermally conductive fillers formed a thermally conductive network on and parallel to a surface of the polymer film. Example 2 (1) 1 g of boron nitride (with a particle size of 10-18 m) was added to 100 g of isopropanol, and ultrasonicated at 100 W for 2 h to obtain a1 wt.% boron nitride dispersion. (2) 5 mL of the boron nitride dispersion was added to 1,000 mL of water. After the boron nitride was evenly dispersed on the water surface, a polyurethane film with a length of 30 cm, a width of 20 cm and a thickness of 0.5 mm was positioned below the water surface obliquely at an angle of 40 with respect to the horizontal direction. The polyurethane film was moved upwards in the oblique direction at a speed of 3 mm/s. At the same time, a stainless steel bar with a width of 25 cm was applied with a force of1 N to push the boron nitride horizontally towards the polyurethane film at a constant speed, so that the boron nitride was attached to the surface of the polyurethane film. (3) The polyurethane film was completely removed from the water and dried at 60°C for min to obtain a boron nitride/polyurethane composite film. (4) 100 turns of the boron nitride/polyurethane composite film were mechanically wound, and then heat treated in an oven at 80°C for 12 h to obtain an anisotropic thermally conductive multilayer polymer composite material. After tests, the obtained composite material was determined to have an in-plane thermal conductivity coefficient of 0.278 W/m-K and a normal thermal conductivity coefficient of 0.06 W/m-K. Example 3 (1) 0.1 g of graphene (with a particle size of 0.1-0.5 m) was added to 100 g of N-methylpyrrolidone, and ultrasonicated at 100 W for 2 h to obtain a 0.1 wt.% graphene dispersion. (2) 10 mL of the graphene dispersion was added to an n-hexane-water system (with 100 mL of n-hexane and 1,000 mL of water). After the graphene was evenly dispersed at the intermediate interface, a silicone rubber film with a length of 50 cm, a width of 30 cm and a thickness of 0.5 mm was positioned below the water surface obliquely at an angle of 40 with respect to the horizontal direction. The silicon rubber was moved upwards in the oblique direction at a speed of 5 mm/s. At the same time, a stainless steel bar with a width of 35 cm was applied with a force of 1.5 N to push the graphene horizontally towards the silicon rubber film at a constant speed, so that the graphene was attached to the surface of the silicone rubber film. (3) The silicone rubber film was completely removed from the water and dried at 60°C for min to obtain a graphene/silicone rubber composite film. (4) The graphene/silicone rubber composite film was cut into strips with a width of 5 mm, manually stacked to achieve 100 layers, and then heat treated in an oven at 150°C for 6 h to obtain an anisotropic thermally conductive multilayer polymer composite material. After tests, the obtained composite material was determined to have an in-plane thermal conductivity coefficient of 9.13 W/m-K and a normal thermal conductivity coefficient of 0.146 W/m-K. Example 4 (1) 0.3 g of carbon nanotube (with a particle size of 70-90 m and an aspect ratio of 500-2,000) was added to 100 g of N,N'-dimethylformamide, ultrasonicated at 100 W for 2 h to obtain a 0.3 wt.% carbon nanotube dispersion. (2) 1 mL of the carbon nanotube dispersion was added to an n-hexane-water system (with 100 mL of n-hexane and 500 mL of water). After the carbon nanotube was evenly dispersed at the intermediate interface, a polyurethane film with a length of 30 cm, a width of 20 cm and a thickness of 0.3 mm was positioned below the water surface obliquely at an angle of 45 with respect to the horizontal direction. The polyurethane film was moved upwards in the oblique direction at a speed of 5 mm/s. At the same time, a stainless steel bar with a width of 25 cm was applied with a force of 0.5 N to push the carbon nanotube horizontally towards the polyurethane flm at a constant speed, so that the carbon nanotube was attached to the surface of the polyurethane film. (3) The polyurethane film was completely removed from the water and dried at 60°C for min to obtain a carbon nanotube/polyurethane composite film. (4) 150 turns of the carbon nanotube/polyurethane composite film were mechanically wound, and then heat treated in an oven at 80°C for 12 h to obtain an anisotropic thermally conductive multilayer polymer composite material. After tests, the obtained composite material was determined to have an in-plane thermal conductivity coefficient of 9.73 W/m-K and a normal thermal conductivity coefficient of 0.08 W/m-K. The above descriptions are merely preferred implementations of the present invention. It should be noted that a person of ordinary skill in the art may further make several improvements and modifications without departing from the principle of the present invention, but such improvements and modifications should be deemed as falling within the protection scope of the present invention.
Claims (5)
- What is claimed is: 1. A method for preparing an anisotropic thermally conductive multilayer polymer composite material, comprising the following steps: step (1): providing a thermally conductive filler dispersion; step (2): adding the thermally conductive filler dispersion to an immiscible two-layer system which comprises an upper layer system as a liquid phase or a gas phase and a lower layer system as a liquid phase, wherein a thermally conductive filler is oriented and dispersed at an intermediate interface of the immiscible two-layer system; step (3): immersing a polymer film in the lower layer system of the immiscible two-layer system containing the thermally conductive filler, moving the polymer film obliquely upward and at the same time pushing the thermally conductive filler horizontally towards the polymer film at a constant speed by using a bar having a width greater than or equal to that of the polymer film, so that the thermally conductive filler is attached to a surface of the polymer film; andremoving the polymer film attached with the thermally conductive filler completely from the immiscible two-layer system to obtain a thermally conductivefiller/polymer composite film; step (4): stacking or winding the thermally conductive filler/polymer composite film, and subjecting to heat treatment to obtain an anisotropic thermally conductive multilayer polymer composite material.
- 2. The method according to claim 1, wherein the thermally conductive filler is one or more of boron nitride, graphite, graphene, carbon nanotube and carbon fiber; a particle size of the thermally conductive filler is 0.01-100 [m; a dispersant of the thermally conductive filler dispersion is one or more of ethanol, isopropanol, N,N'-dimethylformamide and N-methylpyrrolidone; and a mass concentration of the thermally conductive filler in the thermally conductive filler dispersion is 0.1-10%; wherein, the immiscible two-layer system comprises one of n-hexane-water system, cyclohexane-water system, octane-water system, air-water system, acetone-water system and water-carbon tetrachloride system; and a volume ratio of the thermally conductive filler dispersion to the lower layer system of the immiscible two-layer system is (0.001-1):1.
- 3. The method according to claim 1, wherein, a material of the polymer film is one or more of polypropylene, polyethylene, polystyrene, polycarbonate, acrylonitrile styrene butadiene copolymer, polyamide, polyethylene terephthalate, polyphenylene ether, polyphenylene sulfide, rigid polyvinyl chloride, polymethyl methacrylate, polyformaldehyde, polysulfone, polyimide, polytetrafluoroethylene, polytrifluorochloroethylene, polyperfluoroethylene propylene, polybutylene terephthalate, chlorinated polyether, styrene butadiene rubber, nitrile rubber, silicone rubber, butadiene rubber, polyisoprene, ethylene propylene rubber and neoprene; and a thickness of the polymer film is 1 m- 1 cm.
- 4. The method according to claim 1, wherein, an angle between a direction of moving the polymer film obliquely upward and a horizontal direction is 1-90°; a speed of moving the polymer film obliquely upward is 0.001-1 m/s; and a force applied to the bar when pushing the thermally conductive filler is 0.0001-10 N; wherein, a volume percentage of the thermally conductive filler in the thermally conductive filler/polymer composite film is 0.01-90%; wherein, the stacking is carried out with 2-200 layers; or the winding is carried out for 2-200 turns; wherein the heat treatment is carried out at 30-150°C for 2-24 h.
- 5. An anisotropic thermally conductive multilayer polymer composite material prepared by the method according to any of claims 1-4, comprising sequentially stacked multiple layers of thermally conductive filler/polymer composite films, wherein the thermally conductive filler/polymer composite films comprise a polymer film and a thermally conductive filler which forms an oriented thermally conductive network on a surface of the polymer film.
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