High-thermal-conductivity interface material composition and preparation method thereof

Abstract

The invention discloses a high thermal conductivity interface material composition and a preparation method thereof, and belongs to the technical field of thermal conductivity materials. The preparation method comprises the following steps: stirring and mixing the modified polysiloxane resin, the first filler, the second filler, the hydrogen-containing silicone oil, the catalyst, the inhibitor and the coupling agent to obtain a mixture, and curing the mixture to obtain the high-thermal-conductivity interface material composition. The core-shell first filler formed by boron nitride and aluminum oxide is combined with micron aluminum oxide and a plurality of high-heat-conductivity components to achieve a synergistic effect, an efficient heat conduction path is built in the high-heat-conductivity interface material composition, and the overall heat conduction performance is improved; modified polysiloxane resin fluorocarbon bonds and a compact molecular structure form an insulation barrier, and the first filler and the micron alumina are uniformly dispersed in a modified polysiloxane resin matrix to fill gaps, so that multiple insulation barriers are jointly formed, and the high-thermal-conductivity interface material composition has good insulation performance.

Description

Technical Field

[0001] The present invention relates to the technical field of thermal conductive materials, and in particular to a high thermal conductive interface material composition and a preparation method thereof. Background Art

[0002] In many fields such as today's electronic devices, power density continues to rise, heat dissipation problems become more prominent, and the demand for high thermal conductivity interface materials is also increasing. At the same time, the stability and safety required for equipment operation also put forward strict standards for the insulation performance of materials. However, traditional high thermal conductivity interface materials are difficult to achieve an ideal balance between thermal conductivity and insulation performance.

[0003] At present, high thermal conductivity interface materials mainly rely on adding high thermal conductivity fillers such as boron nitride and aluminum oxide to the matrix to improve thermal conductivity. However, these materials have many limitations. On the one hand, it is difficult to build an efficient heat conduction network with a single filler, which limits the overall thermal conductivity and discontinuous thermal conduction path; on the other hand, the filler has poor dispersion in the matrix and is prone to agglomeration, thereby increasing the thermal resistance of the interface. In addition, in high temperature or humid heat environment, the insulation performance of traditional materials is easily affected by environmental factors and is difficult to maintain stability for a long time.

[0004] Specifically, although some materials have a certain degree of thermal conductivity, they have obvious shortcomings in insulation performance. For example, some metal-based thermal conductive materials, due to their good electrical conductivity, will cause serious electrical safety risks when used in electronic equipment with strict insulation requirements. However, the thermal conductivity of most materials with excellent insulation performance is difficult to be satisfactory, and they cannot effectively cope with the growing demand for heat dissipation. Taking common organic polymer insulating materials as an example, their thermal conductivity is usually low, which makes it difficult to meet the heat dissipation requirements of high-power equipment.

[0005] To solve these problems, researchers have tried a variety of methods to improve material performance. For example, adding high thermal conductivity fillers to traditional polymer matrices to enhance thermal conductivity. However, due to the poor compatibility of fillers with the matrix, agglomeration is easily caused, which not only increases thermal resistance but also weakens the effect of improving thermal conductivity. In addition, simply adding fillers may also destroy the original insulating structure of the material, resulting in a decrease in insulation performance.

[0006] Therefore, providing a high thermal conductivity interface material composition with good insulation performance and thermal conductivity is an important problem to be solved in the present invention. Summary of the invention

[0007] In order to solve the problems existing in the prior art, the present invention provides a high thermal conductivity interface material composition and a preparation method thereof. Specifically, the technical solution of the present invention includes the following contents: A method for preparing a high thermal conductivity interface material composition comprises the following steps: The modified polysiloxane resin, the first filler, the second filler, the hydrogen-containing silicone oil, the catalyst, the inhibitor and the coupling agent are stirred and mixed to obtain a mixture, and the mixture is cured to obtain the high thermal conductive interface material composition.

[0008] Furthermore, the preparation method of the modified polysiloxane resin comprises the following steps: In a nitrogen protection environment, hexamethyldisiloxane and fluorine gas undergo a fluorination reaction to obtain fluorodisiloxane; tetramethyltetravinylcyclotetrasiloxane, diethoxy(3-glycidyloxypropyl)methylsilane and a polymerization catalyst undergo a first stirring reaction, and then fluorodisiloxane is added to undergo a second stirring reaction to obtain the modified polysiloxane resin.

[0009] Furthermore, the preparation method of the first filler comprises the following steps: Hexagonal boron nitride and urea are subjected to a grinding reaction to obtain amino boron nitride. Aminated boron nitride and 1,3-dicyclohexylcarbodiimide are subjected to a first mixing reaction, and then pyridine-2,3-dicarboxylic acid is added to undergo a second mixing reaction to obtain an intermediate product A. The intermediate product A and potassium hydroxide are subjected to a third mixing reaction to obtain an intermediate product B. The intermediate product B and aluminum chloride are subjected to a fourth mixing reaction to obtain an intermediate product C. The intermediate product C is subjected to a gradient heating in an oxygen environment to obtain the first filler.

[0010] Furthermore, the fluorination reaction is a progressive fluorination reaction, which is carried out at 26-30 mPa for 180-300 s and then at 31-35 mPa for 90-120 s.

[0011] Furthermore, the weight ratio of the tetramethyltetravinylcyclotetrasiloxane, diethoxy(3-glycidyloxypropyl)methylsilane and fluorodisiloxane is 1:0.24-0.26:0.35-0.38.

[0012] Furthermore, the weight ratio of the tetramethyltetravinylcyclotetrasiloxane to the polymerization catalyst is 1:0.004-0.005.

[0013] Furthermore, the polymerization catalyst is potassium trimethylsilanol or tetramethylammonium hydroxide.

[0014] Furthermore, the first stirring reaction includes a reaction temperature of 105-115° C. and a reaction time of 3-4 h.

[0015] Furthermore, the second stirring reaction includes a reaction temperature of 105-115° C. and a reaction time of 2-3 h.

[0016] Furthermore, the weight ratio of the hexagonal boron nitride to urea is 1:4-5.

[0017] Furthermore, the grinding reaction includes a grinding speed of 300-400 r / min and a grinding time of 48-52 h.

[0018] Furthermore, the weight ratio of the amino boron nitride to 1,3-dicyclohexylcarbodiimide is 1:1.23-1.28.

[0019] Furthermore, the first mixing reaction includes a reaction temperature of 23-25° C. and a reaction time of 10-20 min.

[0020] Furthermore, the weight ratio of the amino boron nitride to pyridine-2,3-dicarboxylic acid is 1:1.19-1.25.

[0021] Furthermore, the second mixed reaction includes a reaction temperature of 23-25° C. and a reaction time of 12-16 h.

[0022] Furthermore, the weight ratio of the intermediate product A to potassium hydroxide is 1:4-5.

[0023] Furthermore, the third mixed reaction includes a reaction temperature of 25-27° C. and a reaction time of 80-100 min.

[0024] Furthermore, the weight ratio of the intermediate product B to aluminum chloride is 1:1.8-2.6.

[0025] Furthermore, the fourth mixed reaction includes a reaction temperature of 25-27° C. and a reaction time of 4-5 h.

[0026] Furthermore, the gradient temperature increase includes reaction at 80° C. for 60 min, reaction at 120° C. for 30 min, reaction at 240° C. for 30 min, and reaction at 360° C. for 30 min.

[0027] Furthermore, the second filler is micron alumina.

[0028] Furthermore, the hydrogen-containing silicone oil is methyl hydrogen-containing silicone oil.

[0029] Furthermore, the catalyst is a Custer platinum catalyst.

[0030] Furthermore, the inhibitor is trimethyltrivinylcyclotrisiloxane or 3-methyl-1-ethynyl-3-ol.

[0031] Furthermore, the coupling agent is silane coupling agent A151 or silane coupling agent A171.

[0032] Furthermore, the stirring and mixing includes a mixing temperature of 50-60° C. and a mixing time of 2-4 hours.

[0033] Furthermore, the curing includes a curing temperature of 100-150° C. and a curing time of 1-3 hours.

[0034] Furthermore, the weight ratio of the modified polysiloxane resin, the first filler, the second filler, the hydrogen-containing silicone oil, the catalyst, the inhibitor and the coupling agent is 80-120: 5-8: 15-20: 10-30: 0.8-1.2: 1-2: 3-5.

[0035] Compared with the prior art, the present invention has the following beneficial effects: (1) The present invention obtains fluorodisiloxane through the fluorination reaction between fluorine gas and hexamethyldisiloxane, and then polymerizes tetramethyltetravinylcyclotetrasiloxane, diethoxy (3-glycidyloxypropyl) methylsilane and fluorodisiloxane to obtain a modified polysiloxane resin rich in carbon-carbon double bonds, epoxy groups and carbon-fluorine bonds; amino boron nitride is obtained by ball milling, and then amino boron nitride and pyridine-2,3-dicarboxylic acid are reacted by amide to obtain an intermediate product A, and the intermediate product A is subjected to an ion exchange reaction to obtain an intermediate product C, and then the intermediate product C is subjected to an oxidation reaction to obtain a first filler, and the first filler is a core-shell structure with boron nitride as a core and aluminum oxide as a shell.

[0036] (2) In the present invention, the core-shell first filler formed by boron nitride and alumina, combined with micron alumina, and multiple high thermal conductivity components work synergistically to build an efficient heat conduction path in the high thermal conductivity interface material composition, thereby improving the overall thermal conductivity performance; at the same time, the amino group in the first filler interacts with the epoxy group in the modified polysiloxane resin, thereby improving the dispersibility of the first filler in the modified polysiloxane resin matrix, reducing thermal resistance, and improving the thermal conductivity of the high thermal conductivity interface material composition.

[0037] (3) The carbon-fluorine bonds and compact molecular structure of the modified polysiloxane resin in the present invention form an insulating barrier, and the first filler and micron alumina are evenly dispersed in the modified polysiloxane resin matrix to fill the gaps, and together form multiple insulating barriers to enable the high thermal conductive interface material composition to have good insulating properties. DETAILED DESCRIPTION

[0038] The technical solution of the present invention will be clearly and completely described below through the embodiments of the present invention. Obviously, the described embodiments are only part of the embodiments of the present invention, not all of the embodiments. Based on the embodiments of the present invention, all other embodiments obtained by those skilled in the art without creative work are within the scope of protection of the present invention.

[0039] Unless otherwise specified, the raw materials and reagents used in the present invention are commercially available or can be prepared by known methods.

[0040] Preparation Example 1 The preparation of modified polysiloxane resin comprises the following steps: In a nitrogen protection environment, hexamethyldisiloxane is placed in a fluorinator, reacted at a pressure of 26 mPa in an environment of 55°C for 180 seconds, and then reacted at a pressure of 31 mPa for 90 seconds to obtain fluorodisiloxane; in a nitrogen protection environment, 10 parts by weight of tetramethyltetravinylcyclotetrasiloxane, 2.4 parts by weight of diethoxy(3-glycidyloxypropyl)methylsilane and 0.04 parts by weight of potassium trimethylsilanol are reacted at 105°C for 3 hours for a first stirring reaction, and after the reaction, 3.5 parts by weight of fluorodisiloxane are added, and the reaction is carried out at 105°C for 2 hours for a second stirring reaction, and after the reaction, the temperature is raised to 150°C and kept for 2 hours, and then vacuum distilled for 1 hour to obtain a modified polysiloxane resin.

[0041] Preparation Example 2 The preparation of modified polysiloxane resin comprises the following steps: In a nitrogen protective environment, hexamethyldisiloxane was placed in a fluorinator, reacted at a pressure of 28 mPa for 220 s at 58°C, and then reacted at a pressure of 32 mPa for 100 s to obtain fluorodisiloxane; in an argon protective environment, 10 parts by weight of tetramethyltetravinylcyclotetrasiloxane, 2.45 parts by weight of diethoxy(3-glycidyloxypropyl)methylsilane and 0.043 parts by weight of potassium trimethylsilanol were reacted at 108°C for 3.3 h for a first stirring reaction, and after the reaction, 3.6 parts by weight of fluorodisiloxane were added, and the reaction was carried out at 108°C for 2.5 h for a second stirring reaction. After the reaction, the temperature was raised to 154°C and kept for 2.2 h, and then the modified polysiloxane resin was obtained by reduced pressure distillation for 1.5 h.

[0042] Preparation Example 3 The preparation of modified polysiloxane resin comprises the following steps: In a nitrogen protective environment, hexamethyldisiloxane was placed in a fluorinator, reacted at a pressure of 28 mPa for 250 s in a 62°C environment, and then reacted at a pressure of 34 mPa for 110 s to obtain fluorodisiloxane; in an argon protective environment, 10 parts by weight of tetramethyltetravinylcyclotetrasiloxane, 2.5 parts by weight of diethoxy(3-glycidyloxypropyl)methylsilane and 0.047 parts by weight of tetramethylammonium hydroxide were reacted at 112°C for 3.8 h for a first stirring reaction, and after the reaction, 3.7 parts by weight of fluorodisiloxane were added, and the reaction was carried out at 112°C for 2.7 h for a second stirring reaction. After the reaction, the temperature was raised to 158°C and kept for 2.5 h, and then reduced pressure distillation was performed for 2.5 h to obtain a modified polysiloxane resin.

[0043] Preparation Example 4 The preparation of modified polysiloxane resin comprises the following steps: In a nitrogen protective environment, hexamethyldisiloxane is placed in a fluorinator, reacted at a pressure of 30 mPa for 300 s in a 65°C environment, and then reacted at a pressure of 35 mPa for 120 s to obtain fluorodisiloxane; in a nitrogen protective environment, 10 parts by weight of tetramethyltetravinylcyclotetrasiloxane, 2.6 parts by weight of diethoxy(3-glycidyloxypropyl)methylsilane and 0.05 parts by weight of tetramethylammonium hydroxide are reacted at 115°C for 4 hours for a first stirring reaction, and after the reaction, 3.8 parts by weight of fluorodisiloxane are added, and the reaction is carried out at 115°C for 3 hours for a second stirring reaction, and after the reaction, the temperature is raised to 160°C and kept for 3 hours, and then reduced pressure distillation is performed for 3 hours to obtain a modified polysiloxane resin.

[0044] Preparation Example 5 The preparation of modified polysiloxane resin comprises the following steps: In a nitrogen protection environment, 10 parts by weight of tetramethyltetravinylcyclotetrasiloxane and 0.05 parts by weight of tetramethylammonium hydroxide are reacted at 115°C for 4 hours for a first stirring reaction. After the reaction, 3.8 parts by weight of hexamethyldisiloxane are added and reacted at 115°C for 3 hours for a second stirring reaction. After the reaction, the temperature is raised to 160°C and kept for 3 hours, and then vacuum distilled for 3 hours to obtain a modified polysiloxane resin.

[0045] Preparation Example 6 The preparation of modified polysiloxane resin comprises the following steps: In a nitrogen protection environment, 10 parts by weight of tetramethyltetravinylcyclotetrasiloxane, 2.6 parts by weight of diethoxy(3-glycidyloxypropyl)methylsilane and 0.05 parts by weight of tetramethylammonium hydroxide are reacted at 115°C for 4 hours for a first stirring reaction. After the reaction, 3.8 parts by weight of hexamethyldisiloxane are added and reacted at 115°C for 3 hours for a second stirring reaction. After the reaction, the temperature is raised to 160°C and kept for 3 hours, and then vacuum distilled for 3 hours to obtain a modified polysiloxane resin.

[0046] Preparation Example 7 The preparation of the first filler comprises the following steps: 10 parts by weight of hexagonal boron nitride and 40 parts by weight of urea are dispersed in 500 parts by weight of isopropanol, ground in a planetary ball mill at a speed of 300 r / min for 48 hours, filtered, washed and dried to obtain amino boron nitride; 10 parts by weight of amino boron nitride and 12.3 parts by weight of 3-dicyclohexylcarbodiimide are dispersed in 500 parts by weight of dichloromethane, reacted at 23°C for 10 minutes to perform a first mixing reaction, and after the reaction, 11.9 parts by weight of pyridine-2,3-dicarboxylic acid are added, reacted at 23°C for 12 hours to perform a second mixing reaction, and after the reaction, filtered, rotary evaporated and purified to obtain intermediate product A; 10 parts by weight of intermediate product Material A and 40 parts by weight of potassium hydroxide are dispersed in 800 parts by weight of deionized water, reacted for 80 minutes in an environment of 25°C for a third mixing reaction, and washed and dried after the reaction to obtain an intermediate product B; 10 parts by weight of intermediate product B and 18 parts by weight of aluminum chloride are dispersed in 600 parts by weight of deionized water, reacted for 4 hours in an environment of 25°C for a fourth mixing reaction, and washed and dried after the reaction to obtain an intermediate product C; the intermediate product C obtained above is reacted at 80°C for 60 minutes, 120°C for 30 minutes, 240°C for 30 minutes, and 360°C for 30 minutes in an oxygen environment by gradient heating to obtain a first filler.

[0047] Preparation Example 8 The preparation of the first filler comprises the following steps: 10 parts by weight of hexagonal boron nitride and 45 parts by weight of urea are dispersed in 500 parts by weight of isopropanol, ground in a planetary ball mill at a speed of 320 r / min for 50 hours, filtered, washed, and dried to obtain amino boron nitride; 10 parts by weight of amino boron nitride and 12.5 parts by weight of 3-dicyclohexylcarbodiimide are dispersed in 500 parts by weight of dichloromethane, reacted at 24° C. for 12 minutes to perform a first mixing reaction, and after the reaction, 12.1 parts by weight of pyridine-2,3-dicarboxylic acid are added, reacted at 24° C. for 14 hours to perform a second mixing reaction, and after the reaction, filtered, rotary evaporated, and purified to obtain an intermediate product A; 10 parts by weight of intermediate product A and 42 parts by weight of potassium hydroxide are dispersed in 800 parts by weight of deionized water, reacted in an environment of 26°C for 90 minutes for a third mixing reaction, and washed and dried after the reaction to obtain an intermediate product B; 10 parts by weight of intermediate product B and 20 parts by weight of aluminum chloride are dispersed in 600 parts by weight of deionized water, reacted in an environment of 26°C for 4.3 hours for a fourth mixing reaction, and washed and dried after the reaction to obtain an intermediate product C; the intermediate product C obtained above is reacted at 80°C for 60 minutes, 120°C for 30 minutes, 240°C for 30 minutes, and 360°C for 30 minutes in an oxygen environment by gradient heating to obtain a first filler.

[0048] Preparation Example 9 The preparation of the first filler comprises the following steps: 10 parts by weight of hexagonal boron nitride and 48 parts by weight of urea are dispersed in 500 parts by weight of isopropanol, ground in a planetary ball mill at a speed of 380 r / min for 50 hours, filtered, washed, and dried to obtain amino boron nitride; 10 parts by weight of amino boron nitride and 12.6 parts by weight of 3-dicyclohexylcarbodiimide are dispersed in 500 parts by weight of dichloromethane, reacted at 24° C. for 17 minutes to perform a first mixing reaction, and after the reaction, 12.3 parts by weight of pyridine-2,3-dicarboxylic acid is added, reacted at 24° C. for 15 hours to perform a second mixing reaction, and after the reaction, filtered, rotary evaporated, and purified to obtain an intermediate product A; 10 parts by weight of intermediate product A and 46 parts by weight of potassium hydroxide are dispersed in 800 parts by weight of deionized water, reacted in an environment of 26°C for 95 minutes for a third mixing reaction, and washed and dried after the reaction to obtain an intermediate product B; 10 parts by weight of intermediate product B and 24 parts by weight of aluminum chloride are dispersed in 600 parts by weight of deionized water, reacted in an environment of 26°C for 4.5 hours for a fourth mixing reaction, and washed and dried after the reaction to obtain an intermediate product C; the intermediate product C obtained above is reacted at 80°C for 60 minutes, 120°C for 30 minutes, 240°C for 30 minutes, and 360°C for 30 minutes in an oxygen environment by gradient heating to obtain a first filler.

[0049] Preparation Example 10 The preparation of the first filler comprises the following steps: 10 parts by weight of hexagonal boron nitride and 50 parts by weight of urea are dispersed in 500 parts by weight of isopropanol, ground in a planetary ball mill at a speed of 400 r / min for 52 hours, filtered, washed, and dried to obtain amino boron nitride; 10 parts by weight of amino boron nitride and 12.8 parts by weight of 3-dicyclohexylcarbodiimide are dispersed in 500 parts by weight of dichloromethane, reacted at 25°C for 20 minutes to perform a first mixing reaction, and after the reaction, 12.5 parts by weight of pyridine-2,3-dicarboxylic acid are added, reacted at 25°C for 16 hours to perform a second mixing reaction, and after the reaction, the intermediate product A is obtained by filtering, rotary evaporation, and purification; 10 parts by weight of intermediate product Material A and 50 parts by weight of potassium hydroxide are dispersed in 800 parts by weight of deionized water, reacted in an environment of 27° C. for 100 minutes for a third mixing reaction, and washed and dried after the reaction to obtain an intermediate product B; 10 parts by weight of intermediate product B and 26 parts by weight of aluminum chloride are dispersed in 600 parts by weight of deionized water, reacted in an environment of 27° C. for 5 hours for a fourth mixing reaction, and washed and dried after the reaction to obtain an intermediate product C; the intermediate product C obtained above is reacted at 80° C. for 60 minutes, 120° C. for 30 minutes, 240° C. for 30 minutes, and 360° C. for 30 minutes in an oxygen environment by gradient heating to obtain a first filler.

[0050] Preparation Example 11 The preparation of the first filler comprises the following steps: 10 parts by weight of hexagonal boron nitride and 50 parts by weight of urea are dispersed in 500 parts by weight of isopropanol, ground in a planetary ball mill at a speed of 400 r / min for 52 hours, filtered, washed, and dried to obtain a first filler.

[0051] Example 1

[0052] The preparation of a high thermal conductive interface material composition comprises the following steps: 80 parts by weight of the modified polysiloxane resin prepared in Preparation Example 1, 5 parts by weight of the first filler prepared in Preparation Example 7, 15 parts by weight of micron alumina, 10 parts by weight of methyl hydrogen silicone oil, 0.8 parts by weight of Custer platinum catalyst, 1 to 2 parts by weight of methyl trivinyl cyclotrisiloxane and 3 to 5 parts by weight of silane coupling agent A151 are stirred and mixed at 50°C for 2 hours to obtain a mixture, the mixture is poured into a mold, and cured at 100°C for 1 hour to obtain a high thermal conductive interface material composition.

[0053] Example 2

[0054] The preparation of a high thermal conductive interface material composition comprises the following steps: 95 parts by weight of the modified polysiloxane resin prepared in Preparation Example 2, 6 parts by weight of the first filler prepared in Preparation Example 8, 17 parts by weight of micron alumina, 15 parts by weight of methyl hydrogen silicone oil, 0.9 parts by weight of Custer platinum catalyst, 1.2 parts by weight of methyl trivinyl cyclotrisiloxane and 3.5 parts by weight of silane coupling agent A151 were stirred and mixed at 53°C for 2.5 hours to obtain a mixture, the mixture was poured into a mold, and cured at 110°C for 1.8 hours to obtain a high thermal conductivity interface material composition.

[0055] Example 3

[0056] The preparation of a high thermal conductive interface material composition comprises the following steps: 80 to 120 parts by weight of the modified polysiloxane resin prepared in Preparation Example 3, 7 parts by weight of the first filler prepared in Preparation Example 9, 18 parts by weight of micron alumina, 25 parts by weight of methyl hydrogen silicone oil, 1.1 parts by weight of Custer platinum catalyst, 1.6 parts by weight of 3-methyl-1-ethynyl-3-ol and 4.2 parts by weight of silane coupling agent A171 were stirred and mixed at 56° C. for 3 h to obtain a mixture, the mixture was poured into a mold, and cured at 130° C. for 2.5 h to obtain a high thermal conductive interface material composition.

[0057] Example 4

[0058] The preparation of a high thermal conductive interface material composition comprises the following steps: 120 parts by weight of the modified polysiloxane resin prepared in Preparation Example 4, 8 parts by weight of the first filler prepared in Preparation Example 10, 20 parts by weight of micron alumina, 30 parts by weight of methyl hydrogen silicone oil, 1.2 parts by weight of Custer platinum catalyst, 2 parts by weight of 3-methyl-1-ethynyl-3-ol and 5 parts by weight of silane coupling agent A171 were stirred and mixed at 60°C for 4 hours to obtain a mixture, the mixture was poured into a mold, and cured at 150°C for 3 hours to obtain a high thermal conductivity interface material composition.

[0059] Comparative Example 1 The preparation of a high thermal conductive interface material composition comprises the following steps: 120 parts by weight of the modified polysiloxane resin prepared in Preparation Example 5, 8 parts by weight of the first filler prepared in Preparation Example 10, 20 parts by weight of micron alumina, 30 parts by weight of methyl hydrogen silicone oil, 1.2 parts by weight of Custer platinum catalyst, 2 parts by weight of 3-methyl-1-ethynyl-3-ol and 5 parts by weight of silane coupling agent A171 were stirred and mixed at 60°C for 4 hours to obtain a mixture, the mixture was poured into a mold, and cured at 150°C for 3 hours to obtain a high thermal conductivity interface material composition.

[0060] Comparative Example 2 The preparation of a high thermal conductive interface material composition comprises the following steps: 120 parts by weight of the modified polysiloxane resin prepared in Preparation Example 6, 8 parts by weight of the first filler prepared in Preparation Example 10, 20 parts by weight of micron alumina, 30 parts by weight of methyl hydrogen silicone oil, 1.2 parts by weight of Custer platinum catalyst, 2 parts by weight of 3-methyl-1-ethynyl-3-ol and 5 parts by weight of silane coupling agent A171 were stirred and mixed at 60°C for 4 hours to obtain a mixture, the mixture was poured into a mold, and cured at 150°C for 3 hours to obtain a high thermal conductivity interface material composition.

[0061] Comparative Example 3 The preparation of a high thermal conductive interface material composition comprises the following steps: 120 parts by weight of the modified polysiloxane resin prepared in Preparation Example 4, 8 parts by weight of the first filler prepared in Preparation Example 11, 20 parts by weight of micron alumina, 30 parts by weight of methyl hydrogen silicone oil, 1.2 parts by weight of Custer platinum catalyst, 2 parts by weight of 3-methyl-1-ethynyl-3-ol and 5 parts by weight of silane coupling agent A171 were stirred and mixed at 60°C for 4 hours to obtain a mixture, the mixture was poured into a mold, and cured at 150°C for 3 hours to obtain a high thermal conductivity interface material composition.

[0062] Comparative Example 4 The preparation of a high thermal conductive interface material composition comprises the following steps: 120 parts by weight of the modified polysiloxane resin prepared in Preparation Example 4, 8 parts by weight of hexagonal boron nitride, 20 parts by weight of micron alumina, 30 parts by weight of methyl hydrogen silicone oil, 1.2 parts by weight of Custer platinum catalyst, 2 parts by weight of 3-methyl-1-ethynyl-3-ol and 5 parts by weight of silane coupling agent A171 were stirred and mixed at 60°C for 4 hours to obtain a mixture, the mixture was poured into a mold, and cured at 150°C for 3 hours to obtain a high thermal conductivity interface material composition.

[0063] Comparative Example 5 The preparation of a high thermal conductive interface material composition comprises the following steps: 120 parts by weight of the modified polysiloxane resin prepared in Preparation Example 4, 8 parts by weight of the first filler prepared in Preparation Example 10, 30 parts by weight of methyl hydrogen silicone oil, 1.2 parts by weight of Custer platinum catalyst, 2 parts by weight of 3-methyl-1-ethynyl-3-ol and 5 parts by weight of silane coupling agent A171 were stirred and mixed at 60°C for 4 hours to obtain a mixture, the mixture was poured into a mold, and cured at 150°C for 3 hours to obtain a high thermal conductivity interface material composition.

[0064] Comparative Example 6 The preparation of a high thermal conductive interface material composition comprises the following steps: 120 parts by weight of the modified polysiloxane resin prepared in Preparation Example 5, 8 parts by weight of the first filler prepared in Preparation Example 11, 30 parts by weight of methyl hydrogen silicone oil, 1.2 parts by weight of Custer platinum catalyst, 2 parts by weight of 3-methyl-1-ethynyl-3-ol and 5 parts by weight of silane coupling agent A171 were stirred and mixed at 60°C for 4 hours to obtain a mixture, the mixture was poured into a mold, and cured at 150°C for 3 hours to obtain a high thermal conductivity interface material composition.

[0065] Comparative Example 7 The preparation of a high thermal conductive interface material composition comprises the following steps: 120 parts by weight of the modified polysiloxane resin prepared in Preparation Example 5, 20 parts by weight of micron alumina, 30 parts by weight of methyl hydrogen silicone oil, 1.2 parts by weight of Custer platinum catalyst, 2 parts by weight of 3-methyl-1-ethynyl-3-ol and 5 parts by weight of silane coupling agent A171 were stirred and mixed at 60°C for 4 hours to obtain a mixture, the mixture was poured into a mold, and cured at 150°C for 3 hours to obtain a high thermal conductivity interface material composition.

[0066] Test example The thermal conductivity and breakdown voltage tests were performed on the high thermal conductivity interface material compositions prepared in Examples 1 to 4 and Comparative Examples 1 to 7.

[0067] Thermal conductivity test: The thermal conductivity of the high thermal conductive interface material compositions prepared in Examples 1 to 4 and Comparative Examples 1 to 7 was measured according to the method specified in ASTM D5470. The measurement results are shown in Table 1. Breakdown voltage test: The thermal conductivity of the high thermal conductive interface material compositions prepared in Examples 1 to 4 and Comparative Examples 1 to 7 was measured according to the method specified in ASTM D149. The measurement results are shown in Table 1.

[0068] Table 1. Thermal conductivity test and breakdown voltage test sample Thermal conductivity (W / m·K) Breakdown voltage (kV / mm) Example 1 7.61 7.18 Example 2 9.42 8.21 Example 3 10.38 11.26 Example 4 12.95 13.65 Comparative Example 1 4.31 4.02 Comparative Example 2 6.81 4.51 Comparative Example 3 4.59 3.46 Comparative Example 4 4.61 2.13 Comparative Example 5 4.52 1.48 Comparative Example 6 3.46 1.15 Comparative Example 7 2.75 0.82 It can be seen from Table 1 that the high thermal conductivity interface material compositions prepared in Examples 1 to 4 all have excellent thermal conductivity, indicating that the high thermal conductivity interface material compositions provided by the present invention have achieved good results in constructing efficient heat conduction paths, and the synergistic effect of multiple components effectively builds a continuous and efficient heat conduction network, so that the high thermal conductivity interface material compositions have good thermal conductivity; the thermal conductivity coefficients of Comparative Examples 1 to 7 are significantly lower than those of Examples 1 to 4, which reflects that the materials that have not been improved by the present invention have obvious deficiencies in thermal conductivity, and the problems of a single filler being difficult to form an efficient heat conduction network and poor filler dispersion limit the overall thermal conductivity.

[0069] The high thermal conductivity interface material compositions prepared in Examples 1 to 4 have good insulation properties. The insulation barrier formed by the carbon-fluorine bonds and the compact molecular structure in the modified polysiloxane resin, as well as the multiple insulation barriers formed by the first filler and the micron alumina uniformly dispersed to fill the gaps, make the high thermal conductivity interface material compositions have good insulation properties. The breakdown voltages of Comparative Examples 1 to 7 are generally lower, and the insulation properties are not as good as those of Examples 1 to 4 of the present invention.

[0070] In summary, the high thermal conductive interface material compositions of Examples 1 to 4 show significant advantages in thermal conductivity and insulation performance, which are better than those of Comparative Examples 1 to 7.

[0071] The above-described embodiments provide a detailed description of the technical solutions and beneficial effects of the present invention. It should be understood that the above description is only a specific embodiment of the present invention and is not intended to limit the present invention. Without departing from the spirit and scope of the present invention, the present invention may have various changes and improvements, which fall within the scope of the present invention to be protected.

Claims

1. A method for preparing a high thermal conductive interface material composition, characterized in that: The preparation method comprises the following steps: The modified polysiloxane resin, the first filler, the second filler, the hydrogen-containing silicone oil, the catalyst, the inhibitor and the coupling agent are stirred and mixed to obtain a mixture, and the mixture is cured to obtain the high thermal conductive interface material composition.

2. A method for preparing a high thermal conductive interface material composition as claimed in claim 1, characterized in that: The preparation method of the modified polysiloxane resin comprises the following steps: In a nitrogen protection environment, hexamethyldisiloxane and fluorine gas undergo a fluorination reaction to obtain fluorodisiloxane; tetramethyltetravinylcyclotetrasiloxane, diethoxy(3-glycidyloxypropyl)methylsilane and a polymerization catalyst undergo a first stirring reaction, and then fluorodisiloxane is added to undergo a second stirring reaction to obtain the modified polysiloxane resin.

3. A method for preparing a high thermal conductive interface material composition as claimed in claim 1, characterized in that: The method for preparing the first filler comprises the following steps: Hexagonal boron nitride and urea are subjected to a grinding reaction to obtain amino boron nitride. Aminated boron nitride and 1,3-dicyclohexylcarbodiimide are subjected to a first mixing reaction, and then pyridine-2,3-dicarboxylic acid is added to undergo a second mixing reaction to obtain an intermediate product A. The intermediate product A and potassium hydroxide are subjected to a third mixing reaction to obtain an intermediate product B. The intermediate product B and aluminum chloride are subjected to a fourth mixing reaction to obtain an intermediate product C. The intermediate product C is subjected to a gradient heating in an oxygen environment to obtain the first filler.

4. A method for preparing a high thermal conductive interface material composition as claimed in claim 2, characterized in that: The polymerization catalyst is potassium trimethylsilanol or tetramethylammonium hydroxide.

5. The method for preparing a high thermal conductive interface material composition according to claim 1, characterized in that: The second filler is micron alumina.

6. A method for preparing a high thermal conductive interface material composition as claimed in claim 1, characterized in that: The hydrogen-containing silicone oil is methyl hydrogen-containing silicone oil.

7. A method for preparing a high thermal conductive interface material composition as claimed in claim 1, characterized in that: The catalyst is a Custer platinum catalyst.

8. The method for preparing a high thermal conductive interface material composition according to claim 1, characterized in that: The inhibitor is trimethyltrivinylcyclotrisiloxane or 3-methyl-1-ethynyl-3-ol.

9. The method for preparing a high thermal conductive interface material composition according to claim 1, characterized in that: The coupling agent is silane coupling agent A151 or silane coupling agent A171.

10. A method for preparing a high thermal conductive interface material composition as claimed in claim 1, characterized in that: The weight ratio of the modified polysiloxane resin, the first filler, the second filler, the hydrogen-containing silicone oil, the catalyst, the inhibitor and the coupling agent is 80-120: 5-8: 15-20: 10-30: 0.8-1.2: 1-2: 3-5.