A high thermal conductive interface material composition and a preparation method thereof

Abstract

The application discloses a high-thermal-conductivity interface material composition and a preparation method thereof, and belongs to the technical field of thermal conductive materials. The preparation method comprises the following steps: stirring and mixing modified polysiloxane resin, a first filler, a second filler, hydrogen-containing silicone oil, a catalyst, an inhibitor and a coupling agent to obtain a mixture, and curing the mixture to obtain the high-thermal-conductivity interface material composition. In the application, the core-shell first filler formed by boron nitride and aluminum oxide, in combination with micron aluminum oxide and the synergistic effect of multiple high-thermal-conductivity components, builds an efficient heat conduction path in the high-thermal-conductivity interface material composition, and improves the overall thermal conductivity. The carbon-fluorine bond and the compact molecular structure of the modified polysiloxane resin form an insulating barrier, the first filler and the micron aluminum oxide are uniformly dispersed in the modified polysiloxane resin matrix, fill the voids, and jointly constitute multiple insulating barriers, so that the high-thermal-conductivity interface material composition has good insulating performance.

Description

TECHNICAL FIELD

[0001] The present application relates to the technical field of heat-conducting materials, and particularly relates to a high-thermal-conductivity interface material composition and a preparation method thereof. BACKGROUND

[0002] In many fields such as electronic devices, the power density continues to rise, and the heat dissipation problem is increasingly prominent, and the demand for high-thermal-conductivity interface materials is also increasing day by day. At the same time, the stability and safety required for device operation also put strict standards on the insulation performance of the materials. However, the 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 in the matrix to improve the thermal conductivity. However, these materials have many limitations. On the one hand, a single filler is difficult to build an efficient heat conduction network, which limits the overall thermal conductivity and makes the thermal conduction path discontinuous. On the other hand, the dispersibility of the filler in the matrix is poor, and agglomeration phenomenon is easily generated, thereby increasing the interface thermal resistance. In addition, in a high-temperature or humid environment, the insulation performance of the traditional materials is easily disturbed by environmental factors, and it is difficult to maintain stability for a long time.

[0004] Specifically, some materials have certain thermal conductivity, but have obvious short boards in the insulation performance. For example, some metal-based thermal conductive materials, due to their good electrical conductivity, will cause serious electrical safety risks when applied to electronic devices with strict insulation requirements. And most of the materials with excellent insulation performance have unsatisfactory thermal conductivity, which cannot effectively cope with the increasing heat dissipation demand. For example, the thermal conductivity of common organic polymer insulating materials is usually low, which is difficult to meet the heat dissipation requirements of high-power devices.

[0005] In order to solve these problems, researchers have tried various means to improve the performance of materials. For example, high-thermal-conductivity fillers are added to the traditional polymer matrix to enhance the thermal conductivity. However, due to the poor compatibility between the filler and the matrix, agglomeration phenomenon is easily caused, which not only increases the thermal resistance, but also weakens the effect of improving the thermal conductivity. In addition, simply adding fillers may also damage the original insulation structure of the material, resulting in a decrease in insulation performance.

[0006] Therefore, it is an important problem to be solved by the present application to provide a high-thermal-conductivity interface material composition with good insulation performance and thermal conductivity. SUMMARY

[0007] In order to solve the problems in the prior art, the present application provides a high-thermal-conductivity interface material composition and a preparation method thereof. Specifically, the technical scheme of the present application includes the following contents:

[0008] A preparation method of a high-thermal-conductivity interface material composition, comprising the following steps:

[0009] 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-conductivity interface material composition.

[0010] Further, the preparation method of the modified polysiloxane resin comprises the following steps:

[0011] In a nitrogen protection environment, hexamethyldisiloxane and fluorine gas are subjected to fluorination reaction to obtain fluorinated disiloxane; tetramethyltetra-vinylcyclotetrasiloxane, diethoxy (3-glycidyloxypropyl) methyl silane and a polymerization catalyst are subjected to first stirring reaction, and then fluorinated disiloxane is added to obtain second stirring reaction to obtain the modified polysiloxane resin.

[0012] Further, the preparation method of the first filler comprises the following steps:

[0013] Hexagonal boron nitride and urea are subjected to grinding reaction to obtain aminated boron nitride, the aminated boron nitride and 1,3-dicyclohexyl carbodiimide are subjected to first mixing reaction, and then pyridine-2,3-dicarboxylic acid is added to obtain second mixing reaction to obtain intermediate product A; intermediate product A and potassium hydroxide are subjected to third mixing reaction to obtain intermediate product B, and intermediate product B and aluminum chloride are subjected to fourth mixing reaction to obtain intermediate product C; the intermediate product C is subjected to gradient temperature rising in an oxygen environment to obtain the first filler.

[0014] Further, the fluorination reaction is progressive fluorination reaction, and after reaction at 26-30 mPa for 180-300 s, reaction is performed at 31-35 mPa for 90-120 s.

[0015] Further, the weight ratio of the tetramethyltetra-vinylcyclotetrasiloxane, diethoxy (3-glycidyloxypropyl) methyl silane and fluorinated disiloxane is 1:0.24-0.26:0.35-0.38.

[0016] Further, the weight ratio of the tetramethyltetra-vinylcyclotetrasiloxane and the polymerization catalyst is 1:0.004-0.005.

[0017] Further, the polymerization catalyst is potassium trimethylsilanolate or tetramethylammonium hydroxide.

[0018] Further, the first stirring reaction comprises reaction temperature 105-115 ℃ and reaction time 3-4 h.

[0019] Further, the second stirring reaction comprises reaction temperature 105-115 ℃ and reaction time 2-3 h.

[0020] Further, the weight ratio of the hexagonal boron nitride and the urea is 1:4-5.

[0021] Further, the grinding reaction includes a grinding rotation speed of 300-400 r / min and a grinding time of 48-52 h.

[0022] Further, the weight ratio of the aminated boron nitride and the 1,3-dicyclohexyl carbodiimide is 1:1.23-1.28.

[0023] Further, the first mixing reaction includes a reaction temperature of 23-25°C and a reaction time of 10-20 min.

[0024] Further, the weight ratio of the aminated boron nitride and the pyridine-2,3-dicarboxylic acid is 1:1.19-1.25.

[0025] Further, the second mixing reaction includes a reaction temperature of 23-25°C and a reaction time of 12-16 h.

[0026] Further, the weight ratio of the intermediate product A and the potassium hydroxide is 1:4-5.

[0027] Further, the third mixing reaction includes a reaction temperature of 25-27°C and a reaction time of 80-100 min.

[0028] Further, the weight ratio of the intermediate product B and the aluminum chloride is 1:1.8-2.6.

[0029] Further, the fourth mixing reaction includes a reaction temperature of 25-27°C and a reaction time of 4-5 h.

[0030] Further, the gradient temperature rise includes a reaction at 80°C for 60 min, a reaction at 120°C for 30 min, a reaction at 240°C for 30 min, and a reaction at 360°C for 30 min.

[0031] Further, the second filler is micron alumina.

[0032] Further, the hydrogen-containing silicone oil is methyl hydrogen silicone oil.

[0033] Further, the catalyst is a Karstedt platinum gold catalyst.

[0034] Further, the inhibitor is trimethyl trivinylcyclosiloxane or 3-methyl-1-ethynyl-3-alcohol.

[0035] Further, the coupling agent is silane coupling agent A151 or silane coupling agent A171.

[0036] Further, the stirring mixing includes a mixing temperature of 50-60°C and a mixing time of 2-4 h.

[0037] Further, the curing includes a curing temperature of 100-150℃ and a curing time of 1-3h.

[0038] Further, 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.

[0039] Compared with the prior art, the present application has the following advantages:

[0040] (1) In the present application, fluorosilane is obtained by fluorination between fluorine and hexamethyldisiloxane, then tetramethyltetraethenylcyclotetrasiloxane, diethoxy(3-glycidyloxypropyl)methylsilane and fluorosilane are polymerized to obtain a modified polysiloxane resin containing abundant carbon-carbon double bonds, epoxy groups and carbon-fluorine bonds; boron nitride is obtained by ball milling method, then the intermediate product A is obtained by amide reaction between the amino boron nitride and pyridine-2,3-dicarboxylic acid, the intermediate product C is obtained by ion exchange reaction of the intermediate product A, and then the first filler is obtained by oxidation reaction of the intermediate product C, the first filler is a core-shell structure with boron nitride as the core and aluminum oxide as the shell.

[0041] (2) In the present application, the core-shell first filler formed by boron nitride and aluminum oxide, combined with micron aluminum oxide, multiple high-thermal-conductivity components synergistically build an efficient heat conduction path in the high-thermal-conductivity interface material composition, improving the overall thermal conductivity; at the same time, the amino groups in the first filler interact with the epoxy groups in the modified polysiloxane resin, improving the dispersibility of the first filler in the modified polysiloxane resin matrix, reducing the thermal resistance and improving the thermal conductivity of the high-thermal-conductivity interface material composition.

[0042] (3) In the present application, the carbon-fluorine bonds and the compact molecular structure of the modified polysiloxane resin form an insulating barrier, the first filler and the micron aluminum oxide are uniformly dispersed in the modified polysiloxane resin matrix, filling the voids and together forming multiple insulating barriers, so that the high-thermal-conductivity interface material composition has good insulating properties. DETAILED DESCRIPTION

[0043] The technical solutions of the present application will be described clearly and completely below through the embodiments of the present application. Obviously, the described embodiments are only a part of the embodiments of the present application, not all the embodiments. Based on the embodiments in the present application, all other embodiments obtained by those skilled in the art without creative labor are within the scope of protection of the present application.

[0044] Unless otherwise specified, the raw materials and reagents used in the present application below are commercially available or can be prepared by known methods.

[0045] Preparation Example 1

[0046] The modified polysiloxane resin is prepared by the following steps:

[0047] In a nitrogen environment, hexamethyl disiloxane is placed in a fluorination instrument, and after reacting at 55°C for 180s at a pressure of 26mPa and then reacting at 31mPa for 90s, fluorinated disiloxane is obtained; in a nitrogen environment, 10 parts by weight of tetramethyl tetra-vinyl cyclosiloxane, 2.4 parts by weight of diethoxy (3-glycidyloxy propyl) methyl silane and 0.04 parts by weight of potassium trimethyl silanol are reacted at 105°C for 3h to perform a first stirring reaction, 3.5 parts by weight of fluorinated disiloxane is added after the reaction is completed, and a second stirring reaction is performed at 105°C for 2h, the reaction is completed, the temperature is raised to 150°C and kept for 2h, and then distilled at reduced pressure for 1h to obtain the modified polysiloxane resin.

[0048] Preparation Example 2

[0049] The modified polysiloxane resin is prepared by the following steps:

[0050] In a nitrogen environment, hexamethyl disiloxane is placed in a fluorination instrument, and after reacting at 58°C for 220s at a pressure of 28mPa and then reacting at 32mPa for 100s, fluorinated disiloxane is obtained; in an argon environment, 10 parts by weight of tetramethyl tetra-vinyl cyclosiloxane, 2.45 parts by weight of diethoxy (3-glycidyloxy propyl) methyl silane and 0.043 parts by weight of potassium trimethyl silanol are reacted at 108°C for 3.3h to perform a first stirring reaction, 3.6 parts by weight of fluorinated disiloxane is added after the reaction is completed, and a second stirring reaction is performed at 108°C for 2.5h, the reaction is completed, the temperature is raised to 154°C and kept for 2.2h, and then distilled at reduced pressure for 1.5h to obtain the modified polysiloxane resin.

[0051] Preparation Example 3

[0052] The modified polysiloxane resin is prepared by the following steps:

[0053] In a nitrogen environment, 10 parts by weight of tetramethyltetra-vinylcyclotetrasiloxane, 2.5 parts by weight of diethoxy (3-glycidyloxypropyl) methyl silane and 0.047 parts by weight of tetramethylammonium hydroxide are stirred at 112°C for 3.8 hours to perform a first stirring reaction, 3.7 parts by weight of fluorosiloxane is added after the reaction is completed, and the mixture is stirred at 112°C for 2.7 hours to perform a second stirring reaction, the temperature is then raised to 158°C and kept for 2.5 hours, and then the mixture is distilled under reduced pressure for 2.5 hours to obtain the modified polysiloxane resin.

[0054] Preparation Example 4

[0055] The preparation of the modified polysiloxane resin comprises the following steps:

[0056] In a nitrogen environment, 10 parts by weight of tetramethyltetra-vinylcyclotetrasiloxane, 2.5 parts by weight of diethoxy (3-glycidyloxypropyl) methyl silane and 0.047 parts by weight of tetramethylammonium hydroxide are stirred at 112°C for 3.8 hours to perform a first stirring reaction, 3.7 parts by weight of fluorosiloxane is added after the reaction is completed, and the mixture is stirred at 112°C for 2.7 hours to perform a second stirring reaction, the temperature is then raised to 158°C and kept for 2.5 hours, and then the mixture is distilled under reduced pressure for 2.5 hours to obtain the modified polysiloxane resin.

[0057] Preparation Example 5

[0058] The preparation of the modified polysiloxane resin comprises the following steps:

[0059] In a nitrogen environment, 10 parts by weight of tetramethyltetra-vinylcyclotetrasiloxane, 2.5 parts by weight of diethoxy (3-glycidyloxypropyl) methyl silane and 0.047 parts by weight of tetramethylammonium hydroxide are stirred at 112°C for 3.8 hours to perform a first stirring reaction, 3.7 parts by weight of fluorosiloxane is added after the reaction is completed, and the mixture is stirred at 112°C for 2.7 hours to perform a second stirring reaction, the temperature is then raised to 158°C and kept for 2.5 hours, and then the mixture is distilled under reduced pressure for 2.5 hours to obtain the modified polysiloxane resin.

[0060] Preparation Example 6

[0061] The preparation of the modified polysiloxane resin comprises the following steps:

[0062] In a nitrogen environment, 10 parts by weight of tetramethyltetra vinyl cyclosiloxane, 2.6 parts by weight of diethoxy (3-glycidyloxypropyl) methyl silane and 0.05 parts by weight of tetramethyl ammonium hydroxide were reacted at 115°C for 4h to carry out a first stirring reaction, 3.8 parts by weight of hexamethyl disiloxane was added and reacted at 115°C for 3h to carry out a second stirring reaction, after the reaction was completed, the temperature was increased to 160°C and kept for 3h, and then distilled under reduced pressure for 3h to obtain the modified polysiloxane resin.

[0063] Preparation Example 7

[0064] The preparation of the first filler includes the following steps:

[0065] 10 parts by weight of hexagonal boron nitride and 40 parts by weight of urea were dispersed in 500 parts by weight of isopropyl alcohol, and after being ground in a planetary ball mill at a speed of 300r / min for 48h, the amino boron nitride was obtained after filtration, washing and drying; 10 parts by weight of the amino boron nitride and 12.3 parts by weight of 3-dicyclohexyl carbodiimide were dispersed in 500 parts by weight of dichloromethane, and reacted at 23°C for 10min to carry out a first mixing reaction, 11.9 parts by weight of pyridine-2,3-dicarboxylic acid was added and reacted at 23°C for 12h to carry out a second mixing reaction, and after the reaction was completed, the intermediate product A was obtained after filtration, rotary evaporation and purification; 10 parts by weight of the intermediate product A and 40 parts by weight of potassium hydroxide were dispersed in 800 parts by weight of deionized water and reacted at 25°C for 80min to carry out a third mixing reaction, and after the reaction was completed, the intermediate product B was obtained after washing and drying; 10 parts by weight of the intermediate product B and 18 parts by weight of aluminum chloride were dispersed in 600 parts by weight of deionized water and reacted at 25°C for 4h to carry out a fourth mixing reaction, and after the reaction was completed, the intermediate product C was obtained after washing and drying; the intermediate product C obtained above was subjected to gradient temperature rising at 80°C for 60min, 120°C for 30min, 240°C for 30min and 360°C for 30min in an oxygen environment to obtain the first filler.

[0066] Preparation Example 8

[0067] The preparation of the first filler includes the following steps:

[0068] 10 parts by weight of hexagonal boron nitride and 45 parts by weight of urea are dispersed in 500 parts by weight of isopropyl alcohol, and after being ground in a planetary ball mill at a rotation speed of 320 r / min for 50 h, the amino boron nitride is obtained after filtration, washing and drying; 10 parts by weight of the amino boron nitride and 12.5 parts by weight of 3-dicyclohexyl carbodiimide are dispersed in 500 parts by weight of dichloromethane, and the first mixed reaction is carried out at 24℃ for 12 min, then 12.1 parts by weight of pyridine-2,3-dicarboxylic acid is added, and the second mixed reaction is carried out at 24℃ for 14 h, then after the reaction is completed, the intermediate product A is obtained after filtration, rotary evaporation and purification; 10 parts by weight of the intermediate product A and 42 parts by weight of potassium hydroxide are dispersed in 800 parts by weight of deionized water, and the third mixed reaction is carried out at 26℃ for 90 min, then after the reaction is completed, the intermediate product B is obtained after washing and drying; 10 parts by weight of the intermediate product B and 20 parts by weight of aluminum chloride are dispersed in 600 parts by weight of deionized water, and the fourth mixed reaction is carried out at 26℃ for 4.3 h, then after the reaction is completed, the intermediate product C is obtained after washing and drying; the above obtained intermediate product C is prepared into the first filler by gradient heating at 80℃ for 60 min, at 120℃ for 30 min, at 240℃ for 30 min and at 360℃ for 30 min in an oxygen environment.

[0069] Preparation Example 9

[0070] The preparation of the first filler comprises the following steps:

[0071] 10 parts by weight of hexagonal boron nitride and 48 parts by weight of urea are dispersed in 500 parts by weight of isopropyl alcohol, and after being ground in a planetary ball mill at a rotation speed of 380 r / min for 50 h, the amino boron nitride is obtained after filtration, washing and drying; 10 parts by weight of the amino boron nitride and 12.6 parts by weight of 3-dicyclohexyl carbodiimide are dispersed in 500 parts by weight of dichloromethane, and the first mixed reaction is carried out at 24℃ for 17 min, then 12.3 parts by weight of pyridine-2,3-dicarboxylic acid is added, and the second mixed reaction is carried out at 24℃ for 15 h, then after the reaction is completed, the intermediate product A is obtained after filtration, rotary evaporation and purification; 10 parts by weight of the intermediate product A and 46 parts by weight of potassium hydroxide are dispersed in 800 parts by weight of deionized water, and the third mixed reaction is carried out at 26℃ for 95 min, then after the reaction is completed, the intermediate product B is obtained after washing and drying; 10 parts by weight of the intermediate product B and 24 parts by weight of aluminum chloride are dispersed in 600 parts by weight of deionized water, and the fourth mixed reaction is carried out at 26℃ for 4.5 h, then after the reaction is completed, the intermediate product C is obtained after washing and drying; the above obtained intermediate product C is prepared into the first filler by gradient heating at 80℃ for 60 min, at 120℃ for 30 min, at 240℃ for 30 min and at 360℃ for 30 min in an oxygen environment.

[0072] Preparation Example 10

[0073] The first filler is prepared by the following steps:

[0074] 10 parts by weight of hexagonal boron nitride and 50 parts by weight of urea are dispersed in 500 parts by weight of isopropyl alcohol, and after being ground in a planetary ball mill at a rotation speed of 400 r / min for 52 h, the first filler is obtained after filtration, washing and drying; 10 parts by weight of the first filler and 12.8 parts by weight of 3-dicyclohexyl carbodiimide are dispersed in 500 parts by weight of dichloromethane, and a first mixing reaction is carried out at 25°C for 20 min; 12.5 parts by weight of pyridine-2,3-dicarboxylic acid is added, and a second mixing reaction is carried out at 25°C for 16 h; after the reaction is completed, the intermediate product A is obtained after filtration, rotary evaporation and purification; 10 parts by weight of the intermediate product A and 50 parts by weight of potassium hydroxide are dispersed in 800 parts by weight of deionized water, and a third mixing reaction is carried out at 27°C for 100 min; after the reaction is completed, the intermediate product B is obtained after washing and drying; 10 parts by weight of the intermediate product B and 26 parts by weight of aluminum chloride are dispersed in 600 parts by weight of deionized water, and a fourth mixing reaction is carried out at 27°C for 5 h; after the reaction is completed, the intermediate product C is obtained after washing and drying; the intermediate product C obtained above is subjected to gradient temperature rising at 80°C for 60 min, at 120°C for 30 min, at 240°C for 30 min and at 360°C for 30 min in an oxygen environment to obtain the first filler.

[0075] Preparation Example 11

[0076] The first filler is prepared by the following steps:

[0077] 10 parts by weight of hexagonal boron nitride and 50 parts by weight of urea are dispersed in 500 parts by weight of isopropyl alcohol, and after being ground in a planetary ball mill at a rotation speed of 400 r / min for 52 h, the first filler is obtained after filtration, washing and drying.

[0078] Example 1

[0079] The high-thermal-conductivity interface material composition is prepared by the following steps:

[0080] 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 micrometer alumina, 10 parts by weight of methyl hydrogen silicone oil, 0.8 parts by weight of Karsted platinum gold catalyst, 1-2 parts by weight of methyl trivinylcyclotrisiloxane and 3-5 parts by weight of silane coupling agent A151 are stirred and mixed at 50°C for 2 h to obtain a mixture, and the mixture is poured into a mold and cured at 100°C for 1 h to obtain the high-thermal-conductivity interface material composition.

[0081] Example 2

[0082] The high-thermal-conductivity interface material composition is prepared by the following steps:

[0083] 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 micrometer alumina, 15 parts by weight of methyl hydrogen silicone oil, 0.9 parts by weight of Karstedt platinum catalyst, 1.2 parts by weight of methyl trivinylcyclotrisiloxane, and 3.5 parts by weight of silane coupling agent A151 were mixed at 53°C for 2.5 hours to obtain a mixture, and the mixture was poured into a mold and cured at 110°C for 1.8 hours to obtain a high thermal conductive interface material composition.

[0084] Example 3

[0085] The high thermal conductive interface material composition was prepared by the following steps:

[0086] 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 micrometer alumina, 25 parts by weight of methyl hydrogen silicone oil, 1.1 parts by weight of Karstedt platinum catalyst, 1.6 parts by weight of 3-methyl-1-ethynyl-3-alcohol, and 4.2 parts by weight of silane coupling agent A171 were mixed at 56°C for 3 hours to obtain a mixture, and the mixture was poured into a mold and cured at 130°C for 2.5 hours to obtain a high thermal conductive interface material composition.

[0087] Example 4

[0088] The high thermal conductive interface material composition was prepared by the following steps:

[0089] 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 micrometer alumina, 30 parts by weight of methyl hydrogen silicone oil, 1.2 parts by weight of Karstedt platinum catalyst, 2 parts by weight of 3-methyl-1-ethynyl-3-alcohol, and 5 parts by weight of silane coupling agent A171 were mixed at 60°C for 4 hours to obtain a mixture, and the mixture was poured into a mold and cured at 150°C for 3 hours to obtain a high thermal conductive interface material composition.

[0090] Comparative Example 1

[0091] The high thermal conductive interface material composition was prepared by the following steps:

[0092] 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 micrometer alumina, 30 parts by weight of methyl hydrogen silicone oil, 1.2 parts by weight of Karstedt platinum catalyst, 2 parts by weight of 3-methyl-1-ethynyl-3-alcohol, and 5 parts by weight of silane coupling agent A171 were mixed at 60°C for 4 hours to obtain a mixture, and the mixture was poured into a mold and cured at 150°C for 3 hours to obtain a high thermal conductive interface material composition.

[0093] Comparative Example 2

[0094] Preparation of the high thermal conductive interface material composition comprising the steps of:

[0095] 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 the micrometer alumina, 30 parts by weight of the methyl hydrogen silicone oil, 1.2 parts by weight of the Karstedt platinum catalyst, 2 parts by weight of 3-methyl-l-ethynyl-3-alcohol, and 5 parts by weight of the silane coupling agent A171 were mixed at 60°C for 4 hours to obtain a mixture, and the mixture was poured into a mold and cured at 150°C for 3 hours to prepare the high thermal conductive interface material composition.

[0096] Comparative Example 3

[0097] Preparation of the high thermal conductive interface material composition comprising the steps of:

[0098] 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 the micrometer alumina, 30 parts by weight of the methyl hydrogen silicone oil, 1.2 parts by weight of the Karstedt platinum catalyst, 2 parts by weight of 3-methyl-l-ethynyl-3-alcohol, and 5 parts by weight of the silane coupling agent A171 were mixed at 60°C for 4 hours to obtain a mixture, and the mixture was poured into a mold and cured at 150°C for 3 hours to prepare the high thermal conductive interface material composition.

[0099] Comparative Example 4

[0100] Preparation of the high thermal conductive interface material composition comprising the steps of:

[0101] 120 parts by weight of the modified polysiloxane resin prepared in Preparation Example 4, 8 parts by weight of the hexagonal boron nitride, 20 parts by weight of the micrometer alumina, 30 parts by weight of the methyl hydrogen silicone oil, 1.2 parts by weight of the Karstedt platinum catalyst, 2 parts by weight of 3-methyl-l-ethynyl-3-alcohol, and 5 parts by weight of the silane coupling agent A171 were mixed at 60°C for 4 hours to obtain a mixture, and the mixture was poured into a mold and cured at 150°C for 3 hours to prepare the high thermal conductive interface material composition.

[0102] Comparative Example 5

[0103] Preparation of the high thermal conductive interface material composition comprising the steps of:

[0104] 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 Karstedt's platinum catalyst, 2 parts by weight of 3-methyl-1-ethynyl-3-ol, and 5 parts by weight of silane coupling agent A171 were mixed at 60°C for 4 hours to obtain a mixture, and the mixture was poured into a mold and cured at 150°C for 3 hours to obtain a high thermal conductive interface material composition.

[0105] Comparative Example 6

[0106] Preparation of a high thermal conductive interface material composition included the following steps:

[0107] 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 Karstedt's platinum catalyst, 2 parts by weight of 3-methyl-1-ethynyl-3-ol, and 5 parts by weight of silane coupling agent A171 were mixed at 60°C for 4 hours to obtain a mixture, and the mixture was poured into a mold and cured at 150°C for 3 hours to obtain a high thermal conductive interface material composition.

[0108] Comparative Example 7

[0109] Preparation of a high thermal conductive interface material composition included the following steps:

[0110] 120 parts by weight of the modified polysiloxane resin prepared in Preparation Example 5, 20 parts by weight of micrometer alumina, 30 parts by weight of methyl hydrogen silicone oil, 1.2 parts by weight of Karstedt's platinum catalyst, 2 parts by weight of 3-methyl-1-ethynyl-3-ol, and 5 parts by weight of silane coupling agent A171 were mixed at 60°C for 4 hours to obtain a mixture, and the mixture was poured into a mold and cured at 150°C for 3 hours to obtain a high thermal conductive interface material composition.

[0111] Test Example

[0112] The high thermal conductive interface material compositions prepared in Examples 1 to 4 and Comparative Examples 1 to 7 were subjected to thermal conductivity performance and breakdown voltage tests.

[0113] Thermal conductivity performance test: The thermal conductivity coefficients of the high thermal conductive interface material compositions prepared in Examples 1 to 4 and Comparative Examples 1 to 7 were measured according to the method specified in ASTM D5470, and the results are shown in Table 1.

[0114] Breakdown voltage test: The thermal conductivity coefficients of the high thermal conductive interface material compositions prepared in Examples 1 to 4 and Comparative Examples 1 to 7 were measured according to the method specified in ASTM D149, and the results are shown in Table 1.

[0115] Table 1. Thermal conductivity performance test and breakdown voltage test

[0116] 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

[0117] As can be seen from Table 1, the high-thermal-conductivity interface material compositions prepared in Examples 1-4 all have excellent thermal conductivity, indicating that the high-thermal-conductivity interface material compositions provided by the present application have achieved good results in constructing efficient heat conduction paths, and the multi-component synergistic effect effectively builds a continuous and efficient heat conduction network, so that the high-thermal-conductivity interface material compositions have good thermal conductivity; the thermal conductivities of Comparative Examples 1-7 are all significantly lower than those of Examples 1-4, which reflects that the materials not improved by the present application have obvious deficiencies in thermal conductivity, and the problems such as the difficulty of single filler in forming an efficient heat conduction network and poor dispersibility of the filler limit the overall thermal conductivity.

[0118] The high-thermal-conductivity interface material compositions prepared in Examples 1-4 have good insulation performance, and the carbon-fluorine bond and the tight molecular structure in the modified polysiloxane resin form an insulation barrier, and the first filler and the micron-sized alumina uniformly dispersed and filled in the voids form a multiple insulation barrier, so that the high-thermal-conductivity interface material compositions have good insulation performance; the breakdown voltages of Comparative Examples 1-7 are generally low, and the insulation performance is not as good as that of Examples 1-4 of the present application.

[0119] In summary, the high-thermal-conductivity interface material compositions of Examples 1-4 have significant advantages in thermal conductivity and insulation performance, which are better than those of Comparative Examples 1-7.

[0120] The above examples have described the technical solutions and beneficial effects of the present application in detail, and it should be understood that the above description is only a specific embodiment of the present application and is not used to limit the present application. Without departing from the spirit and scope of the present application, various changes and improvements can be made to the present application, and these changes and improvements all fall within the scope of the present application.

Claims

1. A method of making a high thermal conductivity interface material composition, characterized by, 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-conductivity interface material composition; The preparation method of the modified polysiloxane resin comprises the following steps: In a nitrogen protection environment, hexamethyldisiloxane and fluorine gas are subjected to fluorination reaction to obtain fluorinated disiloxane; tetramethyltetravinylcyclotetrasiloxane, diethoxy (3-glycidyloxypropyl) methylsilane and a polymerization catalyst are subjected to first stirring reaction, and then fluorinated disiloxane is added and subjected to second stirring reaction to obtain the modified polysiloxane resin; The preparation method of the first filler comprises the following steps: Hexagonal boron nitride and urea are subjected to grinding reaction to obtain aminated boron nitride, the aminated boron nitride and 1,3-dicyclohexyl carbodiimide are subjected to first mixing reaction, and then pyridine-2,3-dicarboxylic acid is added and subjected to second mixing reaction to obtain intermediate product A; intermediate product A and potassium hydroxide are subjected to third mixing reaction to obtain intermediate product B, and intermediate product B and aluminum chloride are subjected to fourth mixing reaction to obtain intermediate product C; intermediate product C is subjected to gradient temperature rising in an oxygen environment to obtain the first filler; and the second filler is micron alumina.

2. The method of claim 1, wherein the high thermal conductivity interface material composition is prepared by mixing the conductive filler and the base material in a weight ratio of 1: 1 to 1:

10. The polymerization catalyst is potassium trimethylsilanolate or tetramethylammonium hydroxide.

3. The method of claim 1, wherein the high thermal conductivity interface material composition is prepared by mixing the conductive filler and the base material in a weight ratio of 1: 1 to 1:

10. The hydrogen-containing silicone oil is methyl hydrogen-containing silicone oil.

4. The method of claim 1, wherein the high thermal conductivity interface material composition is prepared by mixing the conductive filler and the base material in a weight ratio of 1: 1 to 1:

10. The catalyst is Karstedt platinum gold catalyst.

5. The method of claim 1, wherein the high thermal conductivity interface material composition is prepared by mixing the conductive filler and the base material in a weight ratio of 1: 1 to 1:

10. The inhibitor is trimethyltrivinylcyclotrisiloxane or 3-methyl-1-ethynyl-3-alcohol.

6. The method of claim 1, wherein the high thermal conductivity interface material composition is prepared by mixing the conductive filler and the base material in a weight ratio of 1: 1 to 1:

10. The coupling agent is silane coupling agent A151 or silane coupling agent A171.

7. The method of claim 1, wherein the high thermal conductivity interface material composition is prepared by mixing the conductive filler and the base material in a weight ratio of 1: 1 to 1:

10. 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.