阅读说明：本技术 一种不对称型硅油及其制备方法和应用 (Asymmetric silicone oil and preparation method and application thereof ) 是由 封玲珑 王圣 金朝阳 纪学顺 俞涛 张聪颖 杨继朋 杨慧雅 崔焱朝 王庆义 于 2020-12-15 设计创作，主要内容包括：本发明提供一种不对称型硅油及其制备方法和应用,将该不对称硅油用作填料的表面处理剂,用于有机硅导热材料,可以改善填料和有机硅之间的相容性,在添加高含量的填料时能改善填料分散性。所述制备方法,包括如下步骤：1)在有机溶剂存在下,将有机硅氧烷单体与金属烷基化合物或金属硅醇盐以及催化促进剂在10-40℃接触反应1-24h；2)加入封端剂,在10-30℃下进行封端反应,优选反应0.5-5h；然后经水洗、干燥除水和脱溶剂后制得硅-氢封端或硅-乙烯基封端的的中间体；3)将所述中间体与烷氧基硅烷或烷氧基硅油进行硅氢加成反应,制得不对称型硅油。(The invention provides asymmetric silicone oil and a preparation method and application thereof. The preparation method comprises the following steps: 1) in the presence of an organic solvent, an organic siloxane monomer, a metal alkyl compound or metal silicon alkoxide and a catalytic promoter are contacted and reacted for 1 to 24 hours at the temperature of between 10 and 40 ℃; 2) adding a blocking agent, and carrying out blocking reaction at 10-30 ℃, preferably reacting for 0.5-5 h; then washing, drying, removing water and desolventizing to obtain a silicon-hydrogen terminated or silicon-vinyl terminated intermediate; 3) and carrying out hydrosilylation reaction on the intermediate and alkoxy silane or alkoxy silicone oil to prepare the asymmetric silicone oil.)

1. A preparation method of asymmetric silicone oil is characterized by comprising the following steps:

1) in the presence of an organic solvent, an organic siloxane monomer, a metal alkyl compound or metal silicon alkoxide and a catalytic promoter are contacted and reacted for 1 to 24 hours at the temperature of between 10 and 40 ℃;

2) adding a blocking agent, and carrying out blocking reaction at 10-30 ℃, preferably reacting for 0.5-5 h; then washing, drying, removing water and removing a solvent to obtain a silicon-hydrogen terminated or silicon-vinyl terminated intermediate;

3) carrying out hydrosilylation reaction on the intermediate and alkoxy silane or alkoxy silicone oil to prepare asymmetric silicone oil;

in the step 1), the organosiloxane monomer contains a silicon-oxygen six-membered ring structure.

2. The method of claim 1, wherein the organosiloxane monomer is selected from one or more of hexamethylcyclotrisiloxane, 2,4, 6-trivinyl-2, 4, 6-trimethylcyclotrisiloxane, 2,4, 6-trimethyl-2, 4, 6-triphenylcyclotrisiloxane, hexaphenylcyclotrisiloxane, 2,4, 6-trimethyl-2, 4, 6-tris (3,3, 3-trifluoropropyl) cyclotrisiloxane;

and/or the capping agent is selected from silane compounds containing one Si-Cl bond and containing one Si-H bond or one Si-CH ═ CH2 bond, for example from one or more of dimethylchlorosilane, vinyldimethylchlorosilane, methylphenylchlorosilane, diphenylchlorosilane.

3. The process according to claim 1 or 2, wherein the metal alkyl compound is selected from the group consisting of lithium and/or sodium metal alkyl compounds, preferably from one or more of methyllithium, ethyllithium, n-butyllithium, sec-butyllithium and tert-butyllithium;

and/or the metal silicon alkoxide is selected from one or more of lithium trimethylsilanolate, sodium trimethylsilanolate, lithium vinyl dimethylsilanolate and sodium vinyl dimethylsilanolate;

and/or the catalytic promoter is selected from one or more of ethers, amides, esters and other carbonyl organic solvents, preferably from one or more of tetrahydrofuran, N-dimethylformamide and dimethyl sulfoxide;

and/or the alkoxysilane or alkoxysilicone is an alkoxy-containing silane or silicone oil containing a vinyl group or a silyloxy group, preferably selected from vinyltrimethoxysilane, vinyltriethoxysilane, alpha-vinylomega-trimethoxypolydimethylsiloxane, alpha-vinylomega-triethoxypolydimethylsiloxane, trimethoxysilane, triethoxysilane, alpha-hydroomega-trimethoxypolydimethylsiloxane, alpha-hydroomega-triethoxypolydimethylsiloxane, alpha-hexenyltrimethoxysilane, alpha-hexenyltriethoxysilane, alpha-octenyltrimethoxysilane, alpha-octenyltriethoxysilane, p-vinylphenyltrimethoxysilane, p-vinylphenyltriethoxysilane, p-vinylbenzyltriethoxysilane, a-vinylsilyloxy-silane, a-vinyltrimethoxysilane, One or more of p-vinylphenylmethyldimethoxysilane, allylphenyltrimethoxysilane and allylphenyltriethoxysilane.

4. The production method according to any one of claims 1 to 3, wherein in step 1), the volume ratio of the catalyst promoter to the organic solvent is 1:1 to 1: 10;

in the step 2), the molar ratio of the end capping agent to the metal alkyl compound or the metal silicon alkoxide is 1:1-1.5: 1.

5. The preparation method according to any one of claims 1 to 3, wherein the hydrosilylation reaction is performed at a temperature of 50 to 100 ℃ in the presence of a catalyst in step 3), wherein the catalyst is a platinum-element-containing catalyst, and the mass amount of the catalyst in the reaction system in step 3) is 0.5 to 10ppm based on the platinum element in the catalyst; the catalyst is, for example, chloroplatinic acid or a Caster catalyst, preferably a Caster catalyst.

6. An asymmetric silicone oil, characterized in that the asymmetric silicone oil has the following structural formula (I):

wherein each B independently has the following structural formula (II):

y has the following structural formula (III):

z in the structural formula (II) and the structural formula (III) is independently alkylene having 10 or less carbon atoms, such as ethylene group or ethylene phenyl group;

each a is independently an aliphatic hydrocarbon group having 20 or less carbon atoms, such as a methyl group, an ethyl group, a propyl group, a butyl group, or a vinyl group;

each R is¹Each independently an aliphatic hydrocarbon group or an aromatic hydrocarbon group having 4 or less carbon atoms, for example, a methyl group, an ethyl group, a propyl group, a butyl group, a phenyl group, or the like;

R²is ethyl, vinyl, phenyl or trifluoropropyl;

each R is³Each independently an aliphatic hydrocarbon group having 4 or less carbon atoms such as a methyl group, an ethyl group, a propyl group, or an isopropyl group;

each R is⁴Each independently is methyl, ethyl or phenyl;

r in formula (II) or formula (III) is 0-2; in the structural formula (III), k is 1-100, and t is 1-10;

in the structural formula (I), m is 1-1000, n is 0-100, p is 0-100, and q is 0-10.

7. The asymmetric silicone oil according to claim 6, wherein the asymmetric silicone oil is obtained by the production method according to any one of claims 1 to 5.

8. Use of an asymmetric silicone oil obtained by the preparation method according to any one of claims 1 to 5 or an asymmetric silicone oil according to any one of claims 6 to 7, characterized in that the asymmetric silicone oil is used in a heat conductive material as a surface treatment agent for a filler.

9. A silicone heat conductive material composition comprising an alumina filler, decyltrimethoxysilane, a vinyl terminated silicone oil, a hydrogen containing silicone oil, an inhibitor and a catalyst, wherein the silicone heat conductive material composition further comprises an asymmetric silicone oil prepared by the preparation method of any one of claims 1 to 5 or the asymmetric silicone oil of any one of claims 6 to 7;

preferably, the alumina filler is a combination of spherical alumina powder, ellipsoidal alumina powder and random alumina powder, and the mass ratio of the spherical alumina powder to the ellipsoidal alumina powder to the random alumina powder is 4.5-5.5:2.5-3.5: 0.5-1.5; preferably, the mass ratio of the alumina filler in the silicone heat conduction material composition is 85% -95%;

preferably, the mass ratio of the asymmetric silicone oil in the silicone heat-conducting material composition is 0.1% -5%, for example 0.5% -2.5%, preferably 0.8% -2.5%;

preferably, the amount of the inhibitor is 0.03-0.08% of the mass of the organosilicon heat-conducting material composition; preferably, the mass ratios of the decyl trimethoxy silane, the vinyl-terminated silicone oil, the hydrogen-containing silicone oil and the catalyst in the organic silicon heat conduction material composition are respectively 0.2-0.5%, 4-10%, 0.1-0.3% and 0.03-0.08% in sequence.

10. The silicone composition according to claim 9, characterized in that the spherical alumina powder has a median particle size in the range of 20-80 μ ι η, preferably 30-50 μ ι η; the ellipsoidal alumina powder has a median particle size in the range of 5 to 40 μm, preferably 15 to 30 μm; the random alumina powder has a median particle size in the range of 0.1 to 5 μm, preferably 1 to 3 μm.

Technical Field

The invention relates to asymmetric silicone oil, a preparation method thereof and application of the asymmetric silicone oil in a heat conduction/electric conduction material.

Background

Generally, the organic material or the silicone material has a large difference in physicochemical properties from the filler surface, and thus has poor compatibility with each other. In order to improve the compatibility between the organic material or the silicone material and the filler, it is necessary to perform surface treatment on the filler.

In the field of electronic components, such as semiconductors, transistors, integrated circuits, light emitting diodes, etc., which need to operate at a set temperature (e.g., room temperature), the electronic components generate heat during operation, which increases the operating temperature of the electronic components, and if the heat is not dissipated in time, the operating state and the service life of the electronic components are affected.

Generally, heat generated by electronic components is conducted to a heat sink or a heat spreader by using a heat conductive material, so as to dissipate the heat. The organic silicon material has the advantages of good high and low temperature resistance, weather resistance, hydrophobicity, low stress and the like, and is widely applied to heat conduction materials. Common organic silicon heat conducting materials comprise a heat conducting adhesive, a heat conducting gasket, heat conducting silicone grease, heat conducting gel, a heat conducting phase change material and the like.

With the advent of the 5G era, the integration of electronic components has increased, the amount of heat generated has increased dramatically, and higher heat dissipation power is required, and therefore, higher thermal conductivity is required for heat conductive materials. The thermal conductivity of the material is related to the thermal conductivity of the used filler and the filling amount of the selected heat-conducting filler, and the more the heat-conducting filler is, the higher the thermal conductivity of the material is, but the material has increased viscosity, so that the processing performance of the material is deteriorated, and the construction is influenced. Meanwhile, due to poor compatibility of the heat-conducting filler and the organic silicon, the dispersibility of the heat-conducting filler in the organic silicon is poor due to a large amount of the heat-conducting filler, so that the filler is precipitated, the heat conductivity of the material is poor, the thermal resistance is increased due to poor contact between the heat-conducting material and a device or a radiating fin, and the overall performance including mechanical performance is reduced.

In order to solve the above problems, the surface of the filler may be treated with a silane coupling agent to improve the compatibility with silicone, but the obtainable effect is limited. Patent reports (US7329706) use silicone polymers with alkoxy groups as one component in thermally conductive materials to increase their thermal conductivity. However, this treatment agent is a mixture, and the degree of surface treatment of the filler is limited, and a heat conductive material having a high heat conductivity (for example, 4W/m · K) cannot be obtained.

Disclosure of Invention

In view of the above, the present invention provides an asymmetric silicone oil and a preparation method thereof, wherein the asymmetric silicone oil is used as a surface treatment agent for a filler, and is used for a silicone heat conduction material, such that compatibility between the filler and silicone can be improved, and filler dispersibility can be improved when a high content of filler is added.

In order to achieve the purpose, the invention provides the following technical scheme:

the invention provides a preparation method of asymmetric silicone oil on one hand, which comprises the following steps:

1) in the presence of an organic solvent, an organic siloxane monomer (namely a raw material monomer) is contacted with a metal alkyl compound or metal silicon alkoxide and a catalytic promoter for reaction for 1-24h at the temperature of 10-40 ℃;

specifically, in step 1), the raw material monomer may be dissolved in an organic solvent, a metal alkyl compound or a metal silicon alkoxide is added at 10-40 ℃, and after stirring, for example, stirring for 0.5-4h, a catalyst promoter is added for reaction;

2) adding a blocking agent, and carrying out blocking reaction at 10-30 ℃, preferably reacting for 0.5-5 h; then washing, drying, removing water and removing a solvent to obtain a silicon-hydrogen terminated or silicon-vinyl terminated intermediate;

3) carrying out hydrosilylation reaction on the intermediate and alkoxy silane or alkoxy silicone oil to prepare asymmetric silicone oil;

in the step 1), the raw material monomer is a six-membered ring organosiloxane monomer with high ring tension, wherein the raw material monomer contains a silicon-oxygen six-membered ring structure (namely, a six-membered ring formed by-Si-O-).

In a preferred embodiment, the starting monomer is selected from one or more of hexamethylcyclotrisiloxane, 2,4, 6-trivinyl-2, 4, 6-trimethylcyclotrisiloxane, 2,4, 6-trimethyl-2, 4, 6-triphenylcyclotrisiloxane, hexaphenylcyclotrisiloxane, 2,4, 6-trimethyl-2, 4, 6-tris (3,3, 3-trifluoropropyl) cyclotrisiloxane;

the capping agent is selected from silane compounds containing one Si-Cl bond and containing one Si-H bond or one Si-CH ═ CH2 bond, and in some embodiments, the capping agent is selected, for example, from one or more of dimethylchlorosilane, vinyldimethylchlorosilane, methylphenylchlorosilane, diphenylchlorosilane.

In step 1), the metal alkyl compound or the metal silanolate is used as an initiator/catalyst. The metal alkyl compound may be selected from lithium and/or sodium metal alkyl compounds, preferably from one or more of methyllithium, ethyllithium, n-butyllithium, sec-butyllithium and tert-butyllithium; more preferably n-butyllithium.

In a preferred embodiment, the metal silicon alkoxide is selected from one or more of lithium trimethylsilanolate, sodium trimethylsilanolate, lithium vinyldimethylsilanolate and sodium vinyldimethylsilanolate; lithium and/or sodium trimethylsilanolate are preferred.

The catalyst promoter may be selected from one or more of ethers, amides, esters and other carbonyl organic solvents, for example, one or more of tetrahydrofuran, N-dimethylformamide and dimethylsulfoxide is preferable.

The alkoxysilane or alkoxysilicone is a silane or silicone oil containing alkoxy groups and containing vinyl or silyloxy groups, preferably selected from the group consisting of vinyltrimethoxysilane, vinyltriethoxysilane, alpha-vinylω -trimethoxypolydimethylsiloxane, alpha-vinylω -triethoxy-polydimethylsiloxane, trimethoxysilane, triethoxysilane, alpha-hydroω -trimethoxypolydimethylsiloxane, alpha-hydroω -triethoxy-polydimethylsiloxane, alpha-hexenyltrimethoxysilane, alpha-hexenyltriethoxysilane, alpha-octenyltrimethoxysilane, alpha-octenyltriethoxysilane, p-vinylphenyltrimethoxysilane, p-vinylphenyltriethoxysilane, p-vinylphenylsiethoxysilane, a-vinylphenylsilyl-hydroxysilane, a-vinylphenylsilyl-trimethoxysilane, a-vinylphenylsilyl, One or more of p-vinylphenylmethyldimethoxysilane, allylphenyltrimethoxysilane and allylphenyltriethoxysilane.

In step 1), the organic solvent may be one or more selected from aliphatic hydrocarbon, benzene organic solvent or tetrahydrofuran, preferably one or more selected from n-hexane, cyclohexane, n-heptane, toluene, xylene and tetrahydrofuran. Tetrahydrofuran is used as an organic solvent, and plays a role of a catalytic promoter at the same time, so that other catalytic promoters can not be added additionally.

In some embodiments, in step 1), the volume ratio of the catalyst promoter to the organic solvent is 1:1 to 1: 10; preferably 1:1 to 1: 6. By controlling this range, a better equilibrium state of reaction rate and product purity can be achieved.

The amount of the organic solvent is not particularly limited as long as the organic solvent can dissolve at least the monomer, and it is preferable to reduce the amount of the organic solvent as much as possible in order to satisfy the requirement. For example, the mass ratio of the monomer to the organic solvent is 1:1 to 1:3, preferably 1: 1-1:1.5.

In some embodiments, in step 2), the molar ratio of the capping agent to the metal alkyl compound or the metal silicon alkoxide is from 1:1 to 1.5:1, preferably from 1.05:1 to 1.1: 1.

The amount of the raw material monomer and the metal alkyl compound or the metal silicon alkoxide in the system may be determined according to the molecular weight of the target compound, and the ratio of the amount may be controlled, as known to those skilled in the art based on the general technical knowledge in the art, for example, in one example, it is required to obtain a silicone oil having a molecular weight of 2000 and a molar ratio of the metal alkyl compound or the metal silicon alkoxide to the monomer of 1:8 to 1:10, preferably 1:9 to 1: 9.5. In addition, the molar amount of the alkoxysilane or alkoxysilicone used for the completion of the blocking is larger than that of the metal alkyl compound or metal silanolate, which is well known to those skilled in the art, and there is no particular limitation on the amount used so that the completion of the blocking can be achieved. In some embodiments, in step 3), the hydrosilylation reaction: the reaction temperature is 50-100 ℃, the reaction is carried out in the presence of a catalyst, the catalyst is a catalyst containing platinum elements, and the mass usage of the catalyst in the reaction system in the step 3) is 0.5-10ppm calculated by the platinum elements in the catalyst; the catalyst is chosen, for example, from chloroplatinic acid (isopropanol solution) or a Caster catalyst (xylene solution), preferably a Caster catalyst. Based on the preparation method, the single-end functional silicone oil with high purity can be synthesized, and the silicone oil is used as the surface treating agent of the inorganic filler, so that the compatibility of the inorganic filler with organic silicon and other materials can be enhanced, the dispersibility of the filler in a system can be improved, the excellent stability of the filler can be maintained while high-content filler is added into a heat conduction material, and the high-heat-conductivity material can be obtained.

The second aspect of the present invention provides an asymmetric silicone oil, which has the following structural formula (I):

wherein each B independently has the following structural formula (II):

y has the following structural formula (III):

z in the structural formula (II) and the structural formula (III) is independently alkylene having 10 or less carbon atoms, such as ethylene group or ethylene phenyl group;

each a is independently an aliphatic hydrocarbon group having 20 or less carbon atoms, such as a methyl group, an ethyl group, a propyl group, a butyl group, or a vinyl group;

each R is¹Each independently an aliphatic hydrocarbon group or an aromatic hydrocarbon group having 4 or less carbon atoms, for example, a methyl group, an ethyl group, a propyl group, a butyl group, a phenyl group, or the like;

R²is ethyl, vinyl, phenyl or trifluoropropyl;

each R is³Each independently an aliphatic hydrocarbon group having 4 or less carbon atoms, e.g.Methyl, ethyl, propyl or isopropyl;

each R is⁴Each independently is methyl, ethyl or phenyl;

r in formula (II) or formula (III) is 0-2; in the formula (III), k is 1 to 100, for example, 5 to 10, 40 to 50,70 to 80, and the like; t-1-10, e.g., 1-2, 6-7, etc.;

in formula (I), m is 1 to 1000, such as 50 to 260, such as 56 to 254, such as 60 to 70, such as 100-; n is 0 to 100, for example 0, 5 to 10, 25 to 30, etc., p is 0 to 100, for example 0, 5 to 10, 60 to 70, etc., and q is 0 to 10, for example 0, 3 to 5, 7 to 8, etc.

The asymmetric silicone oil with the structural formula (I) can be prepared by the preparation method, and the asymmetric silicone oil with high purity can be obtained by the preparation method.

The third aspect of the present invention further provides an application of the asymmetric silicone oil prepared by the above preparation method or the asymmetric silicone oil of the above structural formula (I), wherein the asymmetric silicone oil is used as a surface treatment agent for the filler in the heat conduction material, so as to improve compatibility between the filler and other components, improve dispersibility of the filler in the silicone, and prepare the high heat conduction material.

The fourth aspect of the present invention also provides a silicone heat-conductive material composition which can include an alumina filler, decyltrimethoxysilane, a vinyl-terminated silicone oil, a hydrogen-containing silicone oil, an inhibitor and a catalyst as in the silicone heat-conductive materials existing in the art, and further, the silicone composition of the present invention further includes the above-described asymmetric silicone oil. The mass ratio of the asymmetric silicone oil in the silicone heat conduction material composition can be 0.1% -5%, preferably 0.5% -2.5%, and further preferably 0.8% -2.5%, and a better application effect can be obtained by adopting a preferable dosage. In some embodiments, the amount of inhibitor used may be, for example, 0.03% to 0.08%, preferably 0.04% to 0.6% of the amount of the silicone heat conductive material composition described above; the amount of the alumina filler is 85 to 95 percent, preferably 88 to 92 percent of the mass of the organic silicon heat conduction material composition; the dosage of the decyl trimethoxy silane is 0.2 to 0.5 percent of the mass of the organic silicon heat conduction material composition; the amount of the vinyl-terminated silicone oil is 4-10%, preferably 8-9.5% of the mass of the organic silicon heat conduction material composition; the dosage of the hydrogen-containing silicone oil is 0.1 to 0.3 percent of the mass of the organic silicon heat conduction material composition; the amount of the catalyst is 0.03-0.08%, preferably 0.04-0.06% of the mass of the organic silicon heat conduction material composition.

Preferably, in the silicone heat-conducting material composition provided by the invention, the alumina filler is a composition of spherical alumina powder, ellipsoidal alumina powder and random alumina powder, and the mass ratio of the spherical alumina powder to the ellipsoidal alumina powder to the random alumina powder is 4.5-5.5:2.5-3.5: 0.5-1.5. The alumina filler formed by combining the alumina powders is matched with the asymmetric silicone oil for use, so that the dispersibility, the hardness and the thermal conductivity of the organic silicon heat conduction material composition can be well considered. In a preferred embodiment, the spherical alumina powder has a median particle size in the range of 20 to 80 μm, preferably 30 to 50 μm; the ellipsoidal alumina powder has a median particle size in the range of 5 to 40 μm, preferably 15 to 30 μm; the random alumina powder has a median particle size in the range of 0.1 to 5 μm, preferably 1 to 3 μm.

In some embodiments, the viscosity of the vinyl-terminated silicone oil ranges from 50cp to 2000cp, preferably from 300 cp to 500 cp; the viscosity range of the hydrogen-containing silicone oil is 1-20cp, preferably 3-10 cp; the above viscosities are the viscosities measured at room temperature with a rotational viscometer, spindle 21).

The organosilicon heat-conducting material composition can be prepared by adopting the existing organosilicon heat-conducting material preparation method, for example, alumina powder is uniformly mixed with asymmetric silicone oil and decyl trimethoxy silane, then the temperature is raised (for example, the temperature is raised to 150 +/-5 ℃) for vacuum stirring, the pressure is lower than-0.09 MPa for example, the stirring time is 60 +/-10 min for example, then the temperature is lowered (for example, the temperature is lowered to below 40 ℃) for vacuum breaking by nitrogen, and then vinyl silicone oil, hydrogen-containing silicone oil, an inhibitor and a catalyst are added for mixing and defoaming. As the inhibitor used, those commonly used in the art can be used, for example, 1-acetylene-1-cyclohexanol, phenylacetylene, 2-ethynylisopropanol and the like. As the catalyst used, those commonly used in the art can be used, for example, Karster catalyst (platinum content: 0.5 wt%), rhodium-based catalyst, etc.

The technical scheme provided by the invention has the following beneficial effects:

by adopting the preparation method of the asymmetric silicone oil provided by the invention, the obtained asymmetric silicone oil has high purity, has better effect when used as a surface treatment agent of the heat-conducting filler in the heat-conducting material, is beneficial to improving the compatibility of the filler and other components, improves the dispersibility of the filler in a system, maintains the high-dosage filler and simultaneously can give consideration to good dispersibility, thereby being beneficial to obtaining the heat-conducting material with good heat conductivity.

Detailed Description

In order to better understand the technical solution of the present invention, the following examples are further provided to illustrate the present invention, but the present invention is not limited to the following examples.

The raw material sources are as follows: 1. hexamethylcyclotrisiloxane, purity > 98%, aladine; 2. n-hexane with the purity of 99 percent and Inokay; 3. tetrahydrofuran, 99% pure, enokay; 4. n-butyllithium solution, 1.6M n-hexane solution, ImmunoKa; 5. dimethylchlorosilane, 96% in purity, and alatin; 6. vinyl trimethoxy silane, 98% purity, Annaiji chemistry; 7. a kast catalyst, a 2% xylene solution, alatin; 8. n, N-dimethylformamide, 99% purity, enokay; 9. vinyldimethylchlorosilane, 97% pure, Sigma-Aldrich.

Example 1

115.80g (0.52mol) of hexamethylcyclotrisiloxane and 180ml of n-hexane are added into a four-neck flask equipped with mechanical stirring, nitrogen, a thermometer and a rubber plug, after all raw material monomers are dissolved, 9.0ml of n-butyllithium solution (1.6M, n-hexane solution) is absorbed by a syringe and added into a reaction flask through the rubber plug; stirring for 1h at normal temperature, adding 30ml tetrahydrofuran, reacting for 6h at 40 ℃, and then cooling to room temperature; 2.0ml of dimethylchlorosilane (the molar ratio of n-butyllithium to dimethylchlorosilane was 1:1.25) was added, stirred at normal temperature for 2 hours, washed with water three times to neutrality, and anhydrous magnesium sulfate was added to the organic phase to dry overnight, followed by rotary evaporation (100 ℃ C., 10mbar) to remove the solvent and the remaining monomers, to give 89.5g of an intermediate.

50g of the intermediate was taken, 2g of vinyltrimethoxysilane and 5. mu.L of a Karster catalyst (platinum element content 1.5ppm) were added, and the mixture was reacted at 60 ℃ for 6 hours, and then rotary evaporation (110 ℃ C., 10mbar) was carried out to remove excess raw material, whereby 50.2g of asymmetric silicone oil was obtained with a yield of 98%.

Product identification information:

nuclear magnetic data¹³C NMR(100MHz,CDCl₃):[d,ppm]＝1.55(-Si(CH₃)₂-O-,),7.81(Si-CH₂-CH2-Si),8.42(Si-CH₂-CH2-Si)13.80(Si-CH₂-CH2-CH2-CH3),17.82(Si-CH₂-CH2-CH2-CH3)25.51(Si-CH₂-CH2-CH2-CH3),26.12(Si-CH₂-CH2-CH2-CH3),50.50(Si-(OCH₃)₃).²⁹Si NMR(80MHz,CDCl₃):[d,ppm]＝7.94(Si-CH₂-CH2-CH2-CH3),7.45(Si-CH₂-CH2-Si(OCH₃)₃),-21.98(Si-(CH₃)₃),-41.70(Si-CH₂-CH2-Si(OCH₃)₃).

The product has the following structure:

example 2

101.67g (0.46mol) of hexamethylcyclotrisiloxane and 110ml of tetrahydrofuran are added into a four-neck flask provided with a mechanical stirrer, nitrogen, a thermometer and a rubber plug, after raw material monomers are completely dissolved, 20ml of sodium trimethylsilanolate solution (1.0M, tetrahydrofuran solution) is absorbed by a syringe, added into a reaction flask through the rubber plug, reacted for 2 hours at 30 ℃, and then cooled to room temperature; 3.2ml of dimethylchlorosilane (the molar ratio of sodium trimethylsilanolate to dimethylchlorosilane is 1:1.4) was added, the mixture was stirred at normal temperature for 2 hours, washed with water three times to neutrality, anhydrous magnesium sulfate was added to the organic phase, the mixture was dried overnight to remove water, and then rotary evaporation was carried out (100 ℃ C., 10mbar) to remove the solvent and the remaining monomers, whereby 92.67g of an intermediate was obtained.

50g of the intermediate was taken, 2g of vinyltrimethoxysilane and 3. mu.L of a Karster catalyst (platinum element content: 0.9ppm) were added, and the mixture was reacted at 60 ℃ for 6 hours, and then rotary evaporation (110 ℃ C., 10mbar) was carried out to remove excess raw material, whereby 50.1g of asymmetric silicone oil was obtained with a yield of 98%.

Product identification information:

nuclear magnetic data¹³C NMR(100MHz,CDCl₃):[d,ppm]＝1.56(-Si(CH₃)₂-O-,),7.82(Si-CH₂-CH2-Si),8.40(Si-CH₂-CH2-Si),50.52(Si-(OCH₃)₃).²⁹Si NMR(80MHz,CDCl₃):[d,ppm]＝7.60(Si-(CH₃)),7.40(Si-CH₂-CH2-Si(OCH₃)₃),-21.95(Si-(CH₃)₃),-41.72(Si-CH₂-CH2-Si(OCH₃)₃).

The specific structure of the product is as follows:

example 3

Adding 100.46g (0.46mol) of hexamethylcyclotrisiloxane and 180ml of n-hexane into a four-neck flask with mechanical stirring, nitrogen, a thermometer and a rubber plug, sucking 20ml of sodium trimethylsilanolate solution (1.0M, tetrahydrofuran solution) by using a syringe after raw material monomers are completely dissolved, and adding the solution into a reaction flask through the rubber plug; stirring for 1h at normal temperature, adding 50ml tetrahydrofuran, reacting for 4h at normal temperature, and then cooling to room temperature; 2.5ml of dimethylchlorosilane (the molar ratio of sodium trimethylsilanolate to dimethylchlorosilane is 1:1.1) was added, stirred at normal temperature for 2 hours, washed with water three times to neutrality, anhydrous magnesium sulfate was added to the organic phase, the mixture was dried overnight to remove water, and then rotary evaporation was carried out (100 ℃ C., 10mbar) to remove the solvent and the remaining monomers, whereby 80.6g of an intermediate was obtained.

50g of the intermediate was taken, 2g of vinyltrimethoxysilane and 10. mu.L of a Karster catalyst (platinum element content: 3ppm) were added, and the mixture was reacted at 60 ℃ for 4 hours, and then rotary evaporation (110 ℃ C., 10mbar) was carried out to remove excess raw material, whereby 50.6g of asymmetric silicone oil was obtained with a yield of 99%.

Product identification information:

nuclear magnetic data¹³C NMR(100MHz,CDCl₃):[d,ppm]＝1.56(-Si(CH₃)₂-O-,),7.82(Si-CH₂-CH2-Si),8.40(Si-CH₂-CH2-Si),50.52(Si-(OCH₃)₃).²⁹Si NMR(80MHz,CDCl₃):[d,ppm]＝7.60(Si-(CH₃)),7.40(Si-CH₂-CH2-Si(OCH₃)₃),-21.95(Si-(CH₃)₃),-41.72(Si-CH₂-CH2-Si(OCH₃)₃).

The specific structure of the product is as follows:

example 4

109.64g (0.49mol) of hexamethylcyclotrisiloxane and 110ml of tetrahydrofuran are added into a four-neck flask with mechanical stirring, nitrogen and a thermometer, 1.86g of lithium trimethylsilanolate is added after raw material monomers are completely dissolved, the mixture is stirred at normal temperature for reaction for 18 hours, then the mixture is cooled to room temperature, 2.4ml of dimethylchlorosilane (the molar ratio of the lithium trimethylsilanolate to the dimethylchlorosilane is 1:1.1) is added, the mixture is stirred at normal temperature for 2 hours, washed for three times to be neutral, anhydrous magnesium sulfate is added into an organic phase, the mixture is dried overnight for dehydration, and then rotary evaporation (100 ℃ and 10mbar) is carried out to remove solvent and residual monomers, thus obtaining 100.12g of an intermediate.

50g of the intermediate was taken, 2g of vinyltrimethoxysilane and 20. mu.L of a Karster catalyst (platinum element content: 6ppm) were added, the mixture was reacted at 60 ℃ for 2 hours, and then rotary evaporation (110 ℃ C., 10mbar) was carried out to remove excess raw materials, whereby 50.1g of an asymmetric silicone oil was obtained, and the yield was 98%.

Product identification information:

nuclear magnetic data¹³C NMR(100MHz,CDCl₃):[d,ppm]＝1.56(-Si(CH₃)₂-O-,),7.82(Si-CH₂-CH2-Si),8.40(Si-CH₂-CH2-Si),50.52(Si-(OCH₃)₃).²⁹Si NMR(80MHz,CDCl₃):[d,ppm]＝7.60(Si-(CH₃)),7.40(Si-CH₂-CH2-Si(OCH₃)₃),-21.95(Si-(CH₃)₃),-41.72(Si-CH₂-CH2-Si(OCH₃)₃).

The specific structure of the product is as follows:

example 5

1185.51g (5.33mol) of hexamethylcyclotrisiloxane, 800ml of n-hexane and 600ml of tetrahydrofuran are added into a four-neck flask with mechanical stirring, nitrogen and a thermometer, 22.25g of lithium trimethylsilanolate is added after raw material monomers are completely dissolved, the mixture is stirred at normal temperature for reaction for 24 hours, then the mixture is cooled to room temperature, 32.98ml of dimethylchlorosilane (the molar ratio of the lithium trimethylsilanolate to the dimethylchlorosilane is 1:1.28) is added, the mixture is stirred at normal temperature for 2 hours, then the mixture is washed with water for three times to be neutral, anhydrous magnesium sulfate is added into an organic phase, the mixture is dried overnight for removing water, and then solvent and residual monomers are removed by rotary evaporation (100 ℃ and 10mbar), thus obtaining an intermediate 1123.56 g.

1088.90g of the above intermediate was taken, 34g of vinyltrimethoxysilane and 34. mu.L of a Karster catalyst (platinum element content: 0.5ppm) were added thereto, and the mixture was reacted at 60 ℃ for 6 hours, followed by rotary evaporation (110 ℃ C., 10mbar) to remove excess raw material, whereby 1075.71g of an asymmetric silicone oil was obtained in 97% yield.

Product identification information:

nuclear magnetic data¹³C NMR(100MHz,CDCl₃):[d,ppm]＝1.56(-Si(CH₃)₂-O-,),7.82(Si-CH₂-CH2-Si),8.40(Si-CH₂-CH2-Si),50.52(Si-(OCH₃)₃).²⁹Si NMR(80MHz,CDCl₃):[d,ppm]＝7.60(Si-(CH₃)),7.40(Si-CH₂-CH2-Si(OCH₃)₃),-21.95(Si-(CH₃)₃),-41.72(Si-CH₂-CH2-Si(OCH₃)₃).

The specific structure of the product is as follows:

example 6

111.24g (0.50mol) of hexamethylcyclotrisiloxane and 180ml of n-hexane are added into a four-neck flask equipped with mechanical stirring, nitrogen, a thermometer and a rubber plug, after raw material monomers are completely dissolved, 9.0ml of n-butyllithium solution (1.6M, n-hexane solution) is absorbed by a syringe and added into a reaction flask through the rubber plug; stirring for 1h at normal temperature, adding 30ml of N, N-dimethylformamide, reacting for 6h at 40 ℃, and then cooling to room temperature; 2.0ml of dimethylchlorosilane (the molar ratio of n-butyllithium to dimethylchlorosilane is 1:1.25) was added, the mixture was stirred at normal temperature for 2 hours, washed with water three times to neutrality, and anhydrous magnesium sulfate was added to the organic phase to dry overnight, followed by rotary evaporation (150 ℃ C., 10mbar) to remove the solvent and the remaining monomers, whereby 100.5g of an intermediate was obtained.

50g of the intermediate was taken, 2g of vinyltrimethoxysilane and 5. mu.L of a Karster catalyst (platinum element content 1.5ppm) were added, and the mixture was reacted at 60 ℃ for 6 hours, and then rotary evaporation (110 ℃ C., 10mbar) was carried out to remove excess raw material, whereby 50.1g of asymmetric silicone oil was obtained with a yield of 98%.

Product identification information:

nuclear magnetic data¹³C NMR(100MHz,CDCl₃):[d,ppm]＝1.55(-Si(CH₃)₂-O-,),7.81(Si-CH₂-CH2-Si),8.43(Si-CH₂-CH2-Si)13.80(Si-CH₂-CH2-CH2-CH3),17.82(Si-CH₂-CH2-CH2-CH3)25.51(Si-CH₂-CH2-CH2-CH3),26.12(Si-CH₂-CH2-CH2-CH3),50.51(Si-(OCH₃)₃).²⁹Si NMR(80MHz,CDCl₃):[d,ppm]＝7.96(Si-CH₂-CH2-CH2-CH3),7.45(Si-CH₂-CH2-Si(OCH₃)₃),-21.98(Si-(CH₃)₃),-41.72(Si-CH₂-CH2-Si(OCH₃)₃).

The product has the following structure:

example 7

111.23g (0.50mol) of hexamethylcyclotrisiloxane and 180ml of n-hexane are added into a four-neck flask equipped with mechanical stirring, nitrogen, a thermometer and a rubber plug, after raw material monomers are completely dissolved, 5.0ml of n-butyllithium solution (1.6M, n-hexane solution) is absorbed by a syringe and added into a reaction flask through the rubber plug; stirring for 1h at normal temperature, adding 30ml of N, N-dimethylformamide, reacting for 6h at 40 ℃, and then cooling to room temperature; 1.4ml of vinyldimethylchlorosilane (molar ratio of n-butyllithium to vinyldimethylchlorosilane is 1:1.25) was added, stirred at normal temperature for 2 hours, washed with water three times to neutrality, and anhydrous magnesium sulfate was added to the organic phase to dry overnight, followed by rotary evaporation (150 ℃ C., 10mbar) to remove the solvent and the remaining monomers, to give 97.5g of an intermediate.

50g of the intermediate was taken, 1.9g of trimethoxysilane and 5. mu.L of a Karster catalyst (platinum element content: 1.5ppm) were added to the intermediate, the mixture was reacted at 60 ℃ for 6 hours, and then excess raw material was removed by rotary evaporation (110 ℃ C., 10mbar), whereby 50.1g of asymmetric silicone oil was obtained with a yield of 98%.

Product identification information:

nuclear magnetic data¹³C NMR(100MHz,CDCl₃):[d,ppm]＝1.56(-Si(CH₃)₂-O-,),7.82(Si-CH₂-CH2-Si),8.41(Si-CH₂-CH2-Si)13.80(Si-CH₂-CH2-CH2-CH3),17.82(Si-CH₂-CH2-CH2-CH3)25.51(Si-CH₂-CH2-CH2-CH3),26.12(Si-CH₂-CH2-CH2-CH3),50.50(Si-(OCH₃)₃).²⁹Si NMR(80MHz,CDCl₃):[d,ppm]＝7.95(Si-CH₂-CH2-CH2-CH3),7.46(Si-CH₂-CH2-Si(OCH₃)₃),-21.98(Si-(CH₃)₃),-41.70(Si-CH₂-CH2-Si(OCH₃)₃).

The product has the following structure:

example 8

115.82g (0.52mol) of hexamethylcyclotrisiloxane and 180ml of n-hexane are added into a four-neck flask with mechanical stirring, nitrogen, a thermometer and a rubber plug, after all raw material monomers are dissolved, 3.0ml of methyllithium solution (1.6M, ether solution) is absorbed by a syringe and added into a reaction flask through the rubber plug; stirring for 1h at normal temperature, adding 30ml tetrahydrofuran, reacting for 6h at 40 ℃, and then cooling to room temperature; 0.6ml of dimethylchlorosilane (the molar ratio of n-butyllithium to dimethylchlorosilane is 1:1.13) was added, the mixture was stirred at normal temperature for 2 hours, washed with water three times to neutrality, and anhydrous magnesium sulfate was added to the organic phase to dry overnight, followed by rotary evaporation (100 ℃ C., 10mbar) to remove the solvent and the remaining monomers, whereby 90.3g of an intermediate was obtained.

50g of the intermediate was taken, 2g of vinyltrimethoxysilane and 5. mu.L of a Karster catalyst (platinum element content 1.5ppm) were added, and the mixture was reacted at 60 ℃ for 6 hours, and then rotary evaporation (110 ℃ C., 10mbar) was carried out to remove excess raw material, whereby 50.2g of asymmetric silicone oil was obtained with a yield of 98%.

Product identification information:

nuclear magnetic data¹³C NMR(100MHz,CDCl₃):[d,ppm]＝1.55(-Si(CH₃)₂-O-,),7.82(Si-CH₂-CH2-Si),8.42(Si-CH₂-CH2-Si),50.52(Si-(OCH₃)₃).²⁹Si NMR(80MHz,CDCl₃):[d,ppm]＝7.61(Si-(CH₃)),7.42(Si-CH₂-CH2-Si(OCH₃)₃),-21.95(Si-(CH₃)₃),-41.72(Si-CH₂-CH2-Si(OCH₃)₃).

The specific structure of the product is as follows:

example 9

The following parts are parts by weight.

500 parts of spherical alumina powder (median particle size of 40 μm), 300 parts of ellipsoidal alumina powder (median particle size of 20 μm), 100 parts of random alumina powder (median particle size of 2 μm), 20 parts of the asymmetric silicone oil prepared in example 1, 3 parts of decyltrimethoxysilane, which are mixed in a 2L double planetary mixer at room temperature for 15min to form a uniform paste, heated to 150 ℃ and stirred in vacuum for 60min at a pressure of less than-0.09 MPa, cooled to below 40 ℃ and vacuumed with nitrogen, then 87 parts of terminal vinyl silicone oil (viscosity 380cP, vinyl content 0.45 wt%), 2 parts of hydrogen silicone oil (viscosity 5cP, silicon hydrogen content 0.75 wt%), 0.5 part of inhibitor (1-acetylene-1-cyclohexanol) and 0.5 part of Kaster catalyst (platinum content 0.5 wt%) are added, mixed at room temperature for 30min and defoamed for 20min, the viscosity of the obtained single-component heat-conducting gel is 400000 mPas, (rotational viscometer, 7#, 2rpm, room temperature test), hardness of 80(Shore 00), and thermal conductivity of 4W/(m.K). The thermal conductivity data referred to herein is measured by the Hot disk test method.

Example 10

The following parts are parts by weight.

500 parts of spherical alumina powder (median particle size of 40 μm), 300 parts of ellipsoidal alumina powder (median particle size of 20 μm), 100 parts of random alumina powder (median particle size of 2 μm), 10 parts of the asymmetric silicone oil of example 1, 3 parts of decyltrimethoxysilane were mixed in a 2L double planetary mixer at room temperature for 15min to a uniform paste, heated to 150 ℃ and vacuum-stirred for 60min at a pressure of less than-0.09 MPa, cooled to below 40 ℃ and vacuum-broken with nitrogen, then 87 parts of terminal vinyl silicone oil (the viscosity is 380cP, the vinyl content is 0.45 wt%) is added, after uniform mixing, 2 parts of hydrogen-containing silicone oil (the viscosity is 5cP, the silicon hydrogen content is 0.75 wt%), 0.5 part of inhibitor (1-acetylene-1-cyclohexanol) and 0.5 part of Kaster catalyst (the platinum content is 0.5 wt%) are added, mixing is carried out at normal temperature for 30min, defoaming is carried out for 20min, and discharging is carried out. The viscosity of the obtained single-component gel is 900000mPa & s (rotational viscometer, 7#, 2rpm, room temperature test), the hardness is 85(shore 00), the thermal conductivity is 4W/(m & K), and the product is placed for one month without obvious oil separation phenomenon.

Example 11

The following parts are parts by weight.

500 parts of spherical alumina powder (median particle size of 40 μm), 300 parts of ellipsoidal alumina powder (median particle size of 20 μm), 100 parts of random alumina powder (median particle size of 2 μm), 5 parts of the asymmetric silicone oil of example 1, 3 parts of decyltrimethoxysilane were mixed in a 2L double planetary mixer at room temperature for 15min to a uniform paste, heated to 150 ℃ and vacuum-stirred for 60min at a pressure of less than-0.09 MPa, cooled to below 40 ℃ and vacuum-broken with nitrogen, then 87 parts of terminal vinyl silicone oil (the viscosity is 380cP, the vinyl content is 0.45 wt%) is added, after uniform mixing, 2 parts of hydrogen-containing silicone oil (the viscosity is 5cP, the silicon hydrogen content is 0.75 wt%), 0.5 part of inhibitor (1-acetylene-1-cyclohexanol) and 0.5 part of Kaster catalyst (the platinum content is 0.5 wt%) are added, mixing is carried out at normal temperature for 30min, defoaming is carried out for 20min, and discharging is carried out. The obtained single-component gel has the viscosity of 1920000mPa & s (measured by a rotary viscometer, 7#, 2rpm and room temperature), the hardness of 87(shore 00), the thermal conductivity of 3.5W/(m & K), and the product is free from oil separation after being placed for one month.

Comparative example 1 (without addition of asymmetric Silicone oil according to the invention)

The following parts are parts by weight.

500 parts of spherical alumina powder (median particle size of 40 μm), 300 parts of ellipsoidal alumina powder (median particle size of 20 μm), 100 parts of random alumina powder (median particle size of 2 μm), 3 parts of decyltrimethoxysilane, mixing in a 2L double planetary mixer at normal temperature for 15min to obtain a uniform paste, heating to 150 deg.C, vacuum stirring for 60min at a pressure of less than-0.09 MPa, cooling to below 40 deg.C, breaking vacuum with nitrogen, then 87 parts of terminal vinyl silicone oil (the viscosity is 380cP, the vinyl content is 0.45 wt%) is added, after uniform mixing, 2 parts of hydrogen-containing silicone oil (the viscosity is 5cP, the silicon hydrogen content is 0.75 wt%), 0.5 part of inhibitor (1-acetylene-1-cyclohexanol) and 0.5 part of Kaster catalyst (the platinum content is 0.5 wt%) are added, mixing is carried out at normal temperature for 30min, defoaming is carried out for 20min, discharging is carried out, the powder is difficult to wrap by the silicone oil, and the product cannot be in a paste shape.

This comparative example is different from examples 6 to 10 in that, without adding the asymmetric silicone oil of the present invention, when the same high content of filler is added, the dispersibility is poor, the compatibility between the components is poor, and finally, a usable product cannot be obtained.

Example 12

The following parts are parts by weight.

500 parts of irregular alumina powder (median particle size of 40 μm), 300 parts of ellipsoidal alumina powder (median particle size of 20 μm), 100 parts of irregular alumina powder (median particle size of 2 μm), 10 parts of the asymmetric silicone oil of example 1, and 3 parts of decyltrimethoxysilane were mixed in a 2L double planetary mixer at room temperature for 15min to a uniform paste, heated to 150 ℃ and vacuum-stirred for 60min at a pressure of less than-0.09 MPa, cooled to below 40 ℃ and vacuum-broken with nitrogen, then 87 parts of terminal vinyl silicone oil (the viscosity is 380cP, the vinyl content is 0.45 wt%) is added, after uniform mixing, 2 parts of hydrogen-containing silicone oil (the viscosity is 5cP, the silicon hydrogen content is 0.75 wt%), 0.5 part of inhibitor (1-acetylene-1-cyclohexanol) and 0.5 part of Kaster catalyst (the platinum content is 0.5 wt%) are added, mixing is carried out at normal temperature for 30min, defoaming is carried out for 20min, and discharging is carried out. The obtained single-component gel has viscosity of more than 2000000 mPas (rotational viscometer, 7#, 2rpm, room temperature test), hardness of 91(shore 00), thermal conductivity of 4W/(m.K), and no oil bleeding after the product is left for one month.

This example is different from example 7 in that a combination of spherical alumina powder, ellipsoidal alumina powder and irregular alumina powder is not used as an alumina filler, and as a result, the viscosity is significantly increased and the hardness is higher than that of example 7. While example 7 can achieve good viscosity, hardness and thermal conductivity at the same time.

Example 13

The following parts are parts by weight.

500 parts of spherical alumina powder (the median particle size of the particles is 40 mu m), 400 parts of ellipsoidal alumina powder (the median particle size of the particles is 20 mu m), 10 parts of asymmetric silicone oil in example 1, 3 parts of decyltrimethoxysilane are mixed in a 2L double planetary mixer at normal temperature for 15min to form a uniform paste, the temperature is increased to 150 ℃, the vacuum stirring is carried out for 60min, the pressure is lower than-0.09 MPa, the temperature is reduced to below 40 ℃, the nitrogen is broken into vacuum, then 87 parts of terminal vinyl silicone oil (the viscosity is 380cP, the vinyl content is 0.45 wt%) are added, 2 parts of hydrogen-containing silicone oil (the viscosity is 5cP, the silicon hydrogen content is 0.75 wt%), 0.5 part of inhibitor (1-acetylene-1-cyclohexanol) and 0.5 part of Kaster catalyst (the platinum content is 0.5 wt%) are added after the uniform mixing, the defoaming. The viscosity of the obtained single-component gel is more than 570000mPa & s (rotation viscometer, 7#, 2rpm, room temperature test), the hardness is 85(shore 00), the thermal conductivity is 3.7W/(m & K), and the product is placed for one month, and obvious oil bleeding phenomenon appears.

This example is different from example 7 in that a combination of spherical alumina powder, ellipsoidal alumina powder and irregular alumina powder is not used as the alumina filler, and although it can obtain a relatively low viscosity and moderate hardness, the thermal conductivity is significantly decreased.

As can be seen from examples 9-13, the addition of the asymmetric silicone oil of the present invention to the heat conductive material composition can improve the compatibility between the filler and the silicone, and can improve the filler dispersibility when a high content of filler is added, smoothly producing a usable product. Further preferably, the heat-conducting filler is preferably an alumina filler formed by combining spherical alumina powder, ellipsoidal alumina powder and irregular alumina powder, and the dosage of the asymmetric silicone oil is preferably 0.8-2.5%, so that the comprehensive performance of the heat-conducting material is favorably improved, and the good viscosity, hardness and heat conductivity are favorably considered.

It will be appreciated by those skilled in the art that modifications or adaptations to the invention may be made in light of the teachings of the present specification. Such modifications or adaptations are intended to be within the scope of the present invention as defined in the claims.