A one-component heat conductive gel comprising hyperbranched phenyl vinyl polysiloxane and a preparation method thereof
By using a self-made hyperbranched phenyl vinyl polysiloxane thermal conductive gel, the problem of balancing resilience and heat resistance in thermal conductive gels under high filling conditions was solved, achieving a synergistic improvement in high thermal conductivity, excellent resilience, and long-term thermal stability.
Patent Information
- Authority / Receiving Office
- CN · China
- Patent Type
- Applications(China)
- Current Assignee / Owner
- GOLOHO POLYMER (JIANGXI) CO LTD
- Filing Date
- 2026-03-31
- Publication Date
- 2026-06-02
Smart Images

Figure CN122127793A_ABST
Abstract
Description
TECHNICAL FIELD
[0001] The present application belongs to the technical field of silicone polymer materials, and particularly relates to a single-component heat-conducting gel containing hyperbranched phenyl vinyl polysiloxane and a preparation method thereof. BACKGROUND
[0002] With the rapid development of electronic devices towards high power density, miniaturization and integration, the heat generated by the internal chips and modules during operation increases dramatically, and effective heat dissipation has become the key to ensuring the reliability and service life of the device. Heat-conducting interface materials, especially heat-conducting gels, are widely used to fill the micro-gaps between heat-generating elements and heat sinks due to their good surface wettability, low contact thermal resistance and certain compliance, and to build an efficient heat conduction path. In addition to high thermal conductivity, an ideal heat-conducting gel also needs to have excellent resilience to adapt to the vibration and thermal expansion and contraction of the device, and long-term heat resistance to ensure stability in high-temperature environments.
[0003] At present, the most direct and effective method to improve the thermal conductivity of heat-conducting gels is to fill a high proportion of heat-conducting fillers, such as aluminum oxide and boron nitride. When the volume fraction of the fillers reaches a certain level, a continuous or mutually contacting heat-conducting network can be formed in the matrix. However, a high filling amount usually significantly increases the viscosity of the composite material, resulting in poor processability, and more importantly, the introduction of a large amount of rigid fillers severely limits the movement of polymer molecular chains, causing the hardness of the material to rise and the resilience and flexibility to decrease significantly, which can easily lead to fatigue failure or interface peeling under long-term stress or thermal cycling.
[0004] In order to improve the flexibility of the high-filling system, the industry usually adopts methods including using low-viscosity silicone oil, adding plasticizers or surface modifying the fillers. These methods can alleviate the problem of increased hardness to some extent, but often at the expense of mechanical strength, migration resistance or long-term thermal stability, and the effect of improving the resilience rate is limited. On the other hand, improving the resilience rate usually requires optimizing the architecture of the crosslinking network, such as by using special structure crosslinking agents or introducing flexible segments. Some studies have tried to use organosilicon compounds with hyperbranched structure as toughening agents or crosslinking agent components, which can increase the distance between crosslinking points by using their three-dimensional structure, thereby enhancing the resilience of the material. This method can indeed effectively improve the resilience rate, but it is still a challenge to ensure the reliability of the material at high temperatures (such as resistance to thermal oxidation and maintaining strength) while achieving high resilience.
[0005] Furthermore, to meet the stringent requirements for high-temperature environmental stability in applications such as automotive electronics and high-power modules, it is often necessary to introduce heat-resistant groups such as phenyl groups into the formulation, for example, using phenyl silicone oil or phenyl-containing polysiloxanes. While the introduction of phenyl groups does help improve the thermal decomposition temperature and anti-aging properties of the material, their significant steric hindrance may affect crosslinking density and crystallization behavior, sometimes even causing changes in the elastic modulus of the material at room temperature, or creating compatibility issues with highly filled systems, thus posing new challenges to balancing overall performance.
[0006] Therefore, in the development of thermally conductive gels, there are complex interrelationships among the three core performance indicators: high thermal conductivity, high resilience, and high heat resistance. Existing technical solutions often focus on optimizing one or two of these properties. For example, they improve thermal conductivity by optimizing the type and gradation of fillers, improve resilience by changing the matrix polymer structure, or enhance thermal stability by introducing heat-resistant groups. However, when simultaneously meeting extremely high thermal conductivity requirements (e.g., exceeding 8.0 W / (m·K)), excellent elastic recovery (e.g., above 85%), and long-term high-temperature resistance (e.g., initial decomposition temperature exceeding 200℃), existing material systems and formulation designs often struggle to achieve synergistic optimization. How to develop a new material composition, starting from molecular structure design, that is well-compatible with high-filler thermally conductive fillers, constructing efficient thermal conduction pathways while not compromising or even synergistically enhancing the resilience and thermal stability of the matrix itself, thus solving the aforementioned performance balance problem in one go, remains a topic worthy of in-depth research in this field. Summary of the Invention
[0007] This application aims to overcome the shortcomings of existing technologies in achieving both high resilience and excellent high-temperature resistance of thermally conductive gels while using high thermal conductivity fillers. Therefore, it provides a single-component thermally conductive gel containing hyperbranched phenyl vinyl polysiloxane and its preparation method.
[0008] To achieve the above-mentioned objectives, the present invention is implemented through the following technical solution: In a first aspect, the present invention provides a one-component thermally conductive gel comprising hyperbranched phenyl vinyl polysiloxane, prepared from raw materials comprising the following components: Prepare 2-15 parts of hyperbranched phenylvinyl polysiloxane. 0.2-2 parts of hydrogen-containing silicone oil, Catalyst 0.1~2 parts, Inhibitor 0.05~0.5 parts, 80-97 parts of thermally conductive filler; of which, The self-made hyperbranched phenyl vinyl polysiloxane is prepared by hydrosilylation reaction of side-hydrogen-containing polysiloxane and terminal vinyl phenyl polysiloxane.
[0009] As shown in the background section, this application addresses a long-standing challenge in the field of thermally conductive gels: when a large amount of thermally conductive filler is used to achieve high thermal conductivity, the resilience and heat resistance of the material often deteriorate significantly. Existing technologies struggle to effectively reconcile these three contradictions. Therefore, instead of employing conventional methods such as simple physical blending or adding general toughening agents, this invention seeks a breakthrough from the source of molecular structure design. It creatively designs and synthesizes a novel polymer—hyperbranched phenylvinyl polysiloxane—possessing both specific functional groups and topological structures, and introduces it as a core component into the formulation system of a single-component thermally conductive gel.
[0010] The "self-made hyperbranched phenyl vinyl polysiloxane" used in this invention is obtained through a specific synthetic route: first, side-containing hydrogen polysiloxane and terminal vinyl phenyl polysiloxane are prepared separately, and then the two are combined through a hydrosilylation reaction. This design allows the final polymer molecule to simultaneously introduce phenyl and vinyl groups and possess a hyperbranched three-dimensional structure. The introduction of phenyl groups aims to improve the thermal stability of the matrix itself; vinyl groups provide reaction sites for subsequent crosslinking with hydrogen-containing silicone oil, constructing an elastic network; while the hyperbranched structure plays multiple key roles. Its abundant branches and large spatial volume can, on the one hand, physically prevent the tight agglomeration between high-proportion thermally conductive filler particles, promoting the uniform dispersion of fillers in the silicone oil matrix, which is beneficial for constructing a more efficient thermally conductive network pathway. On the other hand, its multifunctional characteristics also help to form richer physical or chemical interactions with the filler surface, enhancing interfacial bonding, thereby forming a composite network structure in the matrix that can effectively conduct heat and buffer stress.
[0011] The complete formulation of this invention is formed by combining 2-15 parts of the self-made polymer with 0.2-2 parts of a hydrogen-containing silicone oil crosslinking agent, 0.1-2 parts of a catalyst, 0.05-0.5 parts of an inhibitor, and up to 80-97 parts of a thermally conductive filler. The synergistic effect of this formulation is manifested in the fact that the self-made polymer not only participates in the construction of the crosslinking network as part of the active matrix, but more importantly, its unique hyperbranched structure effectively alleviates the restriction of polymer molecular chain movement by the filler in the presence of a large amount of filler, providing a microstructural possibility for the material to recover its deformation under pressure, thus ensuring high resilience. Simultaneously, the phenyl units in the polymer chain provide intrinsic thermal stability for the entire crosslinking network, making the material less prone to chain segment degradation or network destruction at high temperatures. Therefore, this invention systematically designs multiple aspects, including improving filler dispersion, optimizing interfacial bonding, strengthening the network structure, and enhancing intrinsic heat resistance, by introducing a structurally specially designed polymer.
[0012] The final technical results demonstrate that this solution successfully overcomes the performance contradictions inherent in high-filler systems. The single-component thermally conductive gel prepared by this formulation, while maintaining excellent thermal conductivity, exhibits significantly improved resilience compared to traditional high-filler systems, demonstrating high resilience characteristics. Furthermore, the material's thermal stability is also significantly enhanced, enabling it to withstand higher operating temperatures. Particularly noteworthy is the comparative experiment, which shows that if only ordinary linear vinyl silicone oil or phenyl silicone oil is used to replace the self-made hyperbranched phenyl vinyl polysiloxane, even with identical proportions of other components and fillers, the resilience and heat resistance of the resulting material will significantly decrease. This strongly demonstrates that the self-made polymer with this specific structure plays an irreplaceable key role in this formulation system, and its technical effects exceed the reasonable expectations of those skilled in the art.
[0013] Preferably, the self-made hyperbranched phenyl vinyl polysiloxane has the structure shown in formula (1): Equation (1) Where a,b,n,m=5~70, and the viscosity is 50~1000 mPa·s.
[0014] Preferably, the method for preparing the self-made hyperbranched phenyl vinyl polysiloxane includes the following steps: (1) Tetramethylcyclotetrasiloxane, octamethylcyclotetrasiloxane and hexamethyldisiloxane are subjected to ring-opening polymerization reaction under the action of alkaline catalyst to prepare side-hydrogen-containing polysiloxane; (2) Methylphenylcyclotetrasiloxane, octamethylcyclotetrasiloxane and tetramethyldivinyldisiloxane are subjected to ring-opening polymerization reaction under the action of alkaline catalyst to prepare end vinylphenyl polysiloxane. (3) In the presence of a platinum catalyst, the side-hydrogenated polysiloxane obtained in step (1) and the terminal vinylphenyl polysiloxane obtained in step (2) are subjected to a hydrosilylation reaction to obtain the hyperbranched phenyl vinylpolysiloxane.
[0015] In general, it is a long-standing technical consensus in this field that oxygen and water must be strictly avoided in hydrosilylation reactions. Existing technologies believe that the participation of oxygen and water will inevitably lead to catalyst poisoning, increased side reactions, and product deterioration.
[0016] However, this invention has discovered that those skilled in the art can precisely fine-tune the hydrosilylation reaction kinetics in hyperbranched polymerization by controlling the introduction of trace amounts of oxygen or water, which are traditionally considered harmful. Furthermore, the addition of oxygen or water is not as a reactant, but as a reaction regulator, which can moderately mitigate the initial activity of the platinum catalyst, promoting a more ordered and gradual reaction between the terminal vinylphenyl polysiloxane and multiple active sites on the side hydrogen-containing polysiloxane, thereby facilitating the generation of hyperbranched polymers with more uniform branched structures and more regular molecular chain structures. The reasons are: (1) a trace amount of oxygen or water may selectively and slightly oxidize or modify some of the highly active platinum catalytic centers, forming active species with slightly lower activity but different selectivity. This is equivalent to artificially creating a "catalyst gradient" with different reaction kinetics in the reaction system; (2) in the hyperbranched polymerization of this application, an excessively rapid reaction can easily lead to excessive local crosslinking or gel formation. The introduced micro-regulator can moderately slow down the initial reaction rate, allowing the terminal vinylphenyl polysiloxane to react more uniformly and orderly with multiple Si-H bonds on the side hydrogen-containing polysiloxane. This is beneficial for forming hyperbranched polymers with more uniform branching and more regular molecular structure, and reduces non-ideal branching or cross-linking byproducts caused by "hot spots" formed due to uncontrolled reaction.
[0017] Thermally conductive gels prepared from polymers with superior structures exhibit a more pronounced synergistic improvement in resilience and heat resistance. When incorporated into formulations, they can more effectively synergize with high-filler thermally conductive fillers, creating composite material systems at the molecular scale that simultaneously possess excellent thermal conductivity pathways, efficient stress dissipation networks, and intrinsic thermal stability. More importantly, the gel's long-term thermal aging stability (e.g., performance retention after 1000 hours at 150°C) and resistance to thermal shock may be significantly improved due to the better intrinsic thermal stability and elastic recovery capabilities of the more regularized branched network. Furthermore, moderately relaxing the extremely stringent requirements for anhydrous and oxygen-free conditions may reduce the complexity of equipment and operational difficulties in large-scale production, thereby improving process robustness and repeatability—an unexpected gain with high industrial practical value.
[0018] Preferably, the hydrosilylation reaction in step (3) is carried out in an atmosphere or system containing a trace amount of a reaction modifier, which is oxygen or water.
[0019] Preferably, the reaction modifier is oxygen, which exists in the reaction protective gas at a volume fraction of 10 ppm to 100 ppm.
[0020] Preferably, the reaction regulator is water, which exists in the terminal vinylphenyl polysiloxane raw material at a content of 10 ppm to 50 ppm.
[0021] Preferably, in step (1), the molar ratio of tetramethylcyclotetrasiloxane, octamethylcyclotetrasiloxane and hexamethyldisiloxane is 1~2:1~2:0.01~0.04.
[0022] Preferably, in step (2), the molar ratio of methylphenylcyclotetrasiloxane, octamethylcyclotetrasiloxane and tetramethyldivinyldisiloxane is 1~2:0.5~1:0.01~0.04.
[0023] Preferably, in step (3), the molar ratio of the side-containing hydrogen polysiloxane to the end-vinylphenyl polysiloxane is 1~2:1~1.5.
[0024] Preferably, the raw materials further include methyl silicone oil and / or vinyl silicone oil; and, The amount of methyl silicone oil used is 0-20 parts by weight, and the amount of vinyl silicone oil used is 0-30 parts.
[0025] Preferably, the methyl silicone oil has the structure shown in formula (2): (2); Where n = 0~8000, and viscosity is 50~1000000 mPa·s.
[0026] Methyl silicone oils with viscosities of 50, 100, 1000, 10000, 50000, 100000, and 1000000 mPa·s can be selected as needed.
[0027] Preferably, the vinyl silicone oil structure is as shown in (2): (3) Where n = 0~8000, and viscosity is 50~1000000 mPa·s.
[0028] Vinyl silicone oils with viscosities of 50, 100, 1000, 10000, 50000, 100000, and 1000000 mPa·s can be selected as needed.
[0029] Preferably, the crosslinking agent, catalyst, and inhibitor are hydrogen-containing polymethylsiloxane, 1,3-divinyl-1,1,3,3-tetramethyldisiloxane platinum complex, and 3,5-dimethyl-1-hexyn-3-ol, respectively.
[0030] The hydrogen-containing polymethylsiloxane structure is a terminally hydrogen-containing polymethylsiloxane or a terminally hydrogen-containing polymethylsiloxane, with an H content of 0.05~0.7%, and is one or both of the following structures (4) and (5): H-Si-O-[Si(Me)2-O] z-Si-H (4) H-Si-O-[Si(H)(Me)-O] x -[Si(Me)2-O] y -Si-H (5) Preferably, the thermally conductive filler is a combination of several of the following: spherical alumina, zinc oxide, boron nitride, aluminum nitride, diamond, copper-plated diamond, and graphene.
[0031] Preferably, the thermally conductive filler particle size D50 is 0.001~300 μm.
[0032] Preferably, the additive is one or more of propyltrimethoxysilane, n-hexyltrimethoxysilane, dodecyltrimethoxysilane, hexadecyltrimethoxysilane, octadecyltrimethoxysilane, and alkoxymethoxysilane.
[0033] Secondly, the present invention also provides a method for preparing the single-component thermally conductive gel, which includes the following steps: mixing the self-made hyperbranched phenyl vinyl polysiloxane and thermally conductive filler, and vacuum stirring at 100~130°C; cooling to 40~60°C, adding the hydrogen-containing silicone oil and inhibitor, and vacuum stirring and mixing; finally adding the catalyst, and vacuum stirring and mixing before discharging.
[0034] Preferably, the hardness of the single-component thermal conductive gel is between 60 and 80 oz.
[0035] Preferably, the thermal conductivity of the single-component thermally conductive gel is in the range of 8.0 to 20.0 W / m·K.
[0036] Preferably, the single-component thermal conductive gel has excellent high-temperature resistance. Utilizing the advantages of hyperbranched silicone oil and phenyl silicone oil, its initial decomposition temperature is above 210℃, and the product can be used at temperatures ranging from 180 to 250℃.
[0037] Preferably, the single-component thermally conductive gel has excellent resilience, with a resilience rate of 86-98%.
[0038] Therefore, the present invention has the following beneficial effects: (1) It has a high thermal conductivity, which can effectively conduct heat to meet the heat dissipation requirements of high-power equipment; (2) While filling with a high proportion of thermally conductive fillers, the gel still maintains excellent high resilience and can better adapt to interfacial stress and deformation; furthermore, due to the introduction of phenyl and optimized cross-linking network, the material exhibits good high and low temperature resistance and significantly improves long-term thermal stability. (3) This single-component product also has good processability, making it easy to store and apply. Attached Figure Description
[0039] Figure 1 This is the infrared spectrum of the hyperbranched phenyl vinyl polysiloxane prepared according to the present invention. Detailed Implementation
[0040] The present invention will be further described below with reference to specific embodiments. Those skilled in the art will be able to implement the present invention based on these descriptions. Furthermore, the embodiments of the present invention described below are generally only some, not all, of the embodiments of the present invention. Therefore, all other embodiments obtained by those skilled in the art based on the embodiments of the present invention without inventive effort should fall within the scope of protection of the present invention.
[0041] Example 1 (1) First, add 100 g of tetramethylcyclotetrasiloxane (D4H), 100 g of octamethylcyclotetrasiloxane (D4), and 48.6 g of hexamethyldisiloxane (MM) to a dry 1L reaction flask and dry under vacuum at 100°C for 2 hours. Purge with nitrogen, cool to 60°C, and add 2 ppm of tetramethylammonium hydroxide silanolate (alkali gel). Raise the temperature to 120°C and stir for 6 hours. Gradually raise the temperature to 145~155°C and stir to break down the catalyst for 2 hours. Maintain the temperature at 150°C and remove low-boiling substances under vacuum for 2 hours, finally obtaining a side-containing hydrogen polysiloxane with a yield of 96%.
[0042] (2) First, 100 g of methylphenylcyclotetrasiloxane (D4Ph), 28 g of octamethylcyclotetrasiloxane (D4), and 20.1 g of tetramethyldivinyldisiloxane were added to a dry 1L reaction flask and dried under vacuum at 100°C for 2 hours. Nitrogen gas was introduced, and the temperature was lowered to 60°C. Then, 2 ppm of tetramethylammonium hydroxide silanolate (alkali gel) was added. The temperature was raised to 100~120°C, and the reaction was stirred for 6 hours. The temperature was gradually raised to 150°C, and the reaction was stirred to break down the catalyst for 2 hours. The temperature was maintained at 150°C, and low-boiling substances were removed under vacuum for 2 hours to finally obtain terminal vinylphenyl polysiloxane with a yield of 98%.
[0043] (3) First, add 50 g of the prepared hydrogen-containing polysiloxane and 2 ppm of platinum catalyst to a dry reaction flask, purge with nitrogen, and heat to 90°C. Slowly add 45 g of end-terminated vinylphenyl polysiloxane to the reaction flask over 1 hour. Maintain the temperature at 60°C and stir for 15 hours to finally obtain hyperbranched phenyl vinylpolysiloxane, the infrared spectrum of which is shown below. Figure 1 As shown, the yield is 95%.
[0044] (4) Add 3 parts of hyperbranched phenyl vinyl polysiloxane, 1.5 parts of methyl silicone oil, 1 part of vinyl silicone oil, 0.2 parts of additives, and 95 parts of thermally conductive fillers (including zinc oxide, aluminum oxide, and aluminum nitride) to a dynamic mixer, heat to 120°C, stir evenly, and vacuum stir for 2 hours. Cool to 50°C, add 0.22 parts of hydrogen-containing silicone oil and 0.05 parts of inhibitor, and vacuum stir for 2 hours. Add 0.2 parts of catalyst, vacuum stir for 2 hours, and finally dispense the material.
[0045] Example 2 (1) First, add 100 g of tetramethylcyclotetrasiloxane (D4H), 100 g of octamethylcyclotetrasiloxane (D4), and 48.6 g of hexamethyldisiloxane (MM) to a dry 1L reaction flask and dry under vacuum at 100°C for 2 hours. Purge with nitrogen, cool to 60°C, and add 2 ppm of tetramethylammonium hydroxide silanolate (alkali gel). Raise the temperature to 120°C and stir for 6 hours. Gradually raise the temperature to 145~155°C and stir to break down the catalyst for 2 hours. Maintain the temperature at 150°C and remove low-boiling substances under vacuum for 2 hours, finally obtaining a side-containing hydrogen polysiloxane with a yield of 96%.
[0046] (2) First, 100 g of methylphenylcyclotetrasiloxane (D4Ph), 28 g of octamethylcyclotetrasiloxane (D4), and 20.1 g of tetramethyldivinyldisiloxane were added to a dry 1L reaction flask and dried under vacuum at 100°C for 2 hours. Nitrogen gas was introduced, and the temperature was lowered to 60°C. Then, 2 ppm of tetramethylammonium hydroxide silanolate (alkali gel) was added. The temperature was raised to 100~120°C, and the reaction was stirred for 6 hours. The temperature was gradually raised to 150°C, and the reaction was stirred to break down the catalyst for 2 hours. The temperature was maintained at 150°C, and low-boiling substances were removed under vacuum for 2 hours to finally obtain terminal vinylphenyl polysiloxane with a yield of 98%.
[0047] (3) First, add 50 g of the prepared hydrogen-containing polysiloxane and 2 ppm of platinum catalyst to a dry reaction flask, purge with nitrogen, and heat to 90°C. Slowly add 45 g of end-terminated vinylphenyl polysiloxane to the reaction flask over 1 hour. Maintain the temperature at 60°C and stir for 15 hours to finally obtain hyperbranched phenyl vinylpolysiloxane with a yield of 95%.
[0048] (4) Add 3 parts of hyperbranched phenyl vinyl polysiloxane, 1.5 parts of methyl silicone oil, 1 part of vinyl silicone oil, 0.2 parts of additives, and 95 parts of thermally conductive fillers (including zinc oxide, alumina, and diamond) to a dynamic mixer, heat to 120°C, stir evenly, and vacuum stir for 2 hours. Cool to 50°C, add 0.22 parts of hydrogen-containing silicone oil and 0.05 parts of inhibitor, and vacuum stir for 2 hours. Add 0.2 parts of catalyst, vacuum stir for 2 hours, and finally dispense the material.
[0049] Example 3 (1) First, add 100 g of tetramethylcyclotetrasiloxane (D4H), 100 g of octamethylcyclotetrasiloxane (D4), and 48.6 g of hexamethyldisiloxane (MM) to a dry 1L reaction flask and dry under vacuum at 100°C for 2 hours. Purge with nitrogen, cool to 60°C, and add 2 ppm of tetramethylammonium hydroxide silanolate (alkali gel). Raise the temperature to 120°C and stir for 6 hours. Gradually raise the temperature to 145~155°C and stir to break down the catalyst for 2 hours. Maintain the temperature at 150°C and remove low-boiling substances under vacuum for 2 hours, finally obtaining a side-containing hydrogen polysiloxane with a yield of 96%.
[0050] (2) First, 100 g of methylphenylcyclotetrasiloxane (D4Ph), 28 g of octamethylcyclotetrasiloxane (D4), and 20.1 g of tetramethyldivinyldisiloxane were added to a dry 1L reaction flask and dried under vacuum at 100°C for 2 hours. Nitrogen gas was introduced, and the temperature was lowered to 60°C. Then, 2 ppm of tetramethylammonium hydroxide silanolate (alkali gel) was added. The temperature was raised to 100~120°C, and the reaction was stirred for 6 hours. The temperature was gradually raised to 150°C, and the reaction was stirred to break down the catalyst for 2 hours. The temperature was maintained at 150°C, and low-boiling substances were removed under vacuum for 2 hours to finally obtain terminal vinylphenyl polysiloxane with a yield of 98%.
[0051] (3) First, add 50 g of the prepared hydrogen-containing polysiloxane and 2 ppm of platinum catalyst to a dry reaction flask, purge with nitrogen, and heat to 90°C. Slowly add 45 g of end-terminated vinylphenyl polysiloxane to the reaction flask over 1 hour. Maintain the temperature at 60°C and stir for 15 hours to finally obtain hyperbranched phenyl vinylpolysiloxane with a yield of 95%.
[0052] (4) Add 3 parts of hyperbranched phenyl vinyl polysiloxane, 1.5 parts of methyl silicone oil, 1 part of vinyl silicone oil, 0.2 parts of additives, and 95 parts of thermally conductive fillers (including zinc oxide, aluminum nitride, and diamond) to a dynamic mixer, heat to 120°C, stir evenly, and vacuum stir for 2 hours. Cool to 50°C, add 0.22 parts of hydrogen-containing silicone oil and 0.05 parts of inhibitor, and vacuum stir for 2 hours. Add 0.2 parts of catalyst, vacuum stir for 2 hours, and finally dispense the material.
[0053] Example 4 (1) First, add 100 g of tetramethylcyclotetrasiloxane (D4H), 100 g of octamethylcyclotetrasiloxane (D4), and 48.6 g of hexamethyldisiloxane (MM) to a dry 1L reaction flask and dry under vacuum at 100°C for 2 hours. Purge with nitrogen, cool to 60°C, and add 2 ppm of tetramethylammonium hydroxide silanolate (alkali gel). Raise the temperature to 120°C and stir for 6 hours. Gradually raise the temperature to 145~155°C and stir to break down the catalyst for 2 hours. Maintain the temperature at 150°C and remove low-boiling substances under vacuum for 2 hours, finally obtaining a side-containing hydrogen polysiloxane with a yield of 96%.
[0054] (2) First, 100 g of methylphenylcyclotetrasiloxane (D4Ph), 28 g of octamethylcyclotetrasiloxane (D4), and 20.1 g of tetramethyldivinyldisiloxane were added to a dry 1L reaction flask and dried under vacuum at 100°C for 2 hours. Nitrogen gas was introduced, and the temperature was lowered to 60°C. Then, 2 ppm of tetramethylammonium hydroxide silanolate (alkali gel) was added. The temperature was raised to 100~120°C, and the reaction was stirred for 6 hours. The temperature was gradually raised to 150°C, and the reaction was stirred to break down the catalyst for 2 hours. The temperature was maintained at 150°C, and low-boiling substances were removed under vacuum for 2 hours to finally obtain terminal vinylphenyl polysiloxane with a yield of 98%.
[0055] (3) First, add 50 g of the prepared hydrogen-containing polysiloxane and 2 ppm of platinum catalyst to a dry reaction flask, purge with nitrogen, and heat to 90°C. Slowly add 45 g of end-terminated vinylphenyl polysiloxane to the reaction flask over 1 hour. Maintain the temperature at 60°C and stir for 15 hours to finally obtain hyperbranched phenyl vinylpolysiloxane with a yield of 95%.
[0056] (4) Add 3 parts of hyperbranched phenyl vinyl polysiloxane, 1.5 parts of methyl silicone oil, 1 part of vinyl silicone oil, 0.2 parts of additives, and 95 parts of thermally conductive fillers (including boron nitride, aluminum nitride, and diamond) to a dynamic mixer, heat to 120°C, stir evenly, and vacuum stir for 2 hours. Cool to 50°C, add 0.22 parts of hydrogen-containing silicone oil and 0.05 parts of inhibitor, and vacuum stir for 2 hours. Add 0.2 parts of catalyst, vacuum stir for 2 hours, and finally dispense the material.
[0057] Example 5 (1) First, add 100 g of tetramethylcyclotetrasiloxane (D4H), 100 g of octamethylcyclotetrasiloxane (D4), and 48.6 g of hexamethyldisiloxane (MM) to a dry 1L reaction flask and dry under vacuum at 100°C for 2 hours. Purge with nitrogen, cool to 60°C, and add 2 ppm of tetramethylammonium hydroxide silanolate (alkali gel). Raise the temperature to 120°C and stir for 6 hours. Gradually raise the temperature to 145~155°C and stir to break down the catalyst for 2 hours. Maintain the temperature at 150°C and remove low-boiling substances under vacuum for 2 hours, finally obtaining a side-containing hydrogen polysiloxane with a yield of 96%.
[0058] (2) First, 100 g of methylphenylcyclotetrasiloxane (D4Ph), 28 g of octamethylcyclotetrasiloxane (D4), and 20.1 g of tetramethyldivinyldisiloxane were added to a dry 1L reaction flask and dried under vacuum at 100°C for 2 hours. Nitrogen gas was introduced, and the temperature was lowered to 60°C. Then, 2 ppm of tetramethylammonium hydroxide silanolate (alkali gel) was added. The temperature was raised to 100~120°C, and the reaction was stirred for 6 hours. The temperature was gradually raised to 150°C, and the reaction was stirred to break down the catalyst for 2 hours. The temperature was maintained at 150°C, and low-boiling substances were removed under vacuum for 2 hours to finally obtain terminal vinylphenyl polysiloxane with a yield of 98%.
[0059] (3) First, add 50 g of the prepared hydrogen-containing polysiloxane and 2 ppm of platinum catalyst to a dry reaction flask, purge with nitrogen, and heat to 90°C. Slowly add 45 g of end-terminated vinylphenyl polysiloxane to the reaction flask over 1 hour. Maintain the temperature at 60°C and stir for 15 hours to finally obtain hyperbranched phenyl vinylpolysiloxane with a yield of 95%.
[0060] (4) Add 3 parts of hyperbranched phenyl vinyl polysiloxane, 1.5 parts of methyl silicone oil, 1 part of vinyl silicone oil, 0.2 parts of additives, and 96 parts of thermally conductive fillers (including boron nitride, aluminum nitride, diamond, and graphene) to a dynamic mixer, heat to 120°C, stir evenly, and vacuum stir for 2 hours. Cool to 50°C, add 0.22 parts of hydrogen-containing silicone oil and 0.05 parts of inhibitor, and vacuum stir for 2 hours. Add 0.2 parts of catalyst, vacuum stir for 2 hours, and finally dispense the material.
[0061] Example 6 (1) First, add 100 g of tetramethylcyclotetrasiloxane (D4H), 100 g of octamethylcyclotetrasiloxane (D4), and 48.6 g of hexamethyldisiloxane (MM) to a dry 1L reaction flask and dry under vacuum at 100°C for 2 hours. Purge with nitrogen, cool to 60°C, and add 2 ppm of tetramethylammonium hydroxide silanolate (alkali gel). Raise the temperature to 120°C and stir for 6 hours. Gradually raise the temperature to 145~155°C and stir to break down the catalyst for 2 hours. Maintain the temperature at 150°C and remove low-boiling substances under vacuum for 2 hours, finally obtaining a side-containing hydrogen polysiloxane with a yield of 96%.
[0062] (2) First, 100 g of methylphenylcyclotetrasiloxane (D4Ph), 28 g of octamethylcyclotetrasiloxane (D4), and 20.1 g of tetramethyldivinyldisiloxane were added to a dry 1L reaction flask and dried under vacuum at 100°C for 2 hours. Nitrogen gas was introduced, and the temperature was lowered to 60°C. Then, 2 ppm of tetramethylammonium hydroxide silanolate (alkali gel) was added. The temperature was raised to 100~120°C, and the reaction was stirred for 6 hours. The temperature was gradually raised to 150°C, and the reaction was stirred to break down the catalyst for 2 hours. The temperature was maintained at 150°C, and low-boiling substances were removed under vacuum for 2 hours to finally obtain terminal vinylphenyl polysiloxane with a yield of 98%.
[0063] (3) First, add 50 g of the prepared hydrogen-containing polysiloxane and 2 ppm of platinum catalyst to a dry reaction flask, purge with nitrogen, and heat to 90°C. Slowly add 45 g of end-terminated vinylphenyl polysiloxane to the reaction flask over 1 hour. Maintain the temperature at 60°C and stir for 15 hours to finally obtain hyperbranched phenyl vinylpolysiloxane with a yield of 95%.
[0064] (4) Add 3 parts of hyperbranched phenyl vinyl polysiloxane, 1.5 parts of methyl silicone oil, 1 part of vinyl silicone oil, 0.2 parts of additives, and 96 parts of thermally conductive fillers (including boron nitride, aluminum nitride, diamond, graphene, and copper-plated diamond) to a dynamic mixer, heat to 120°C, stir evenly, and vacuum stir for 2 hours. Cool to 50°C, add 0.22 parts of hydrogen-containing silicone oil and 0.05 parts of inhibitor, and vacuum stir for 2 hours. Add 0.2 parts of catalyst, vacuum stir for 2 hours, and finally dispense the material.
[0065] Example 7 The preparation of hyperbranched phenyl vinyl polysiloxane is carried out according to steps (1) and (2) of Example 1.
[0066] (3) Preparation of hyperbranched phenyl vinyl polysiloxane First, 50g of the prepared hydrogen-containing polysiloxane and 2ppm of platinum catalyst were added to a dry reaction flask. Nitrogen gas containing 20ppm (volume fraction) of oxygen was introduced into the reaction system as a protective and reaction atmosphere, and the temperature was raised to 90℃. Then, 45g of vinylphenyl polysiloxane was slowly added dropwise to the reaction flask over a period of 1 hour. The mixture was kept at 90℃ and stirred for 15 hours to finally obtain hyperbranched phenyl vinylpolysiloxane.
[0067] (4) Preparation of single-component thermally conductive gel: 3 parts of the obtained hyperbranched phenyl vinyl polysiloxane, 1.5 parts of methyl silicone oil, 1 part of vinyl silicone oil, 0.2 parts of additives, and 95 parts of thermally conductive fillers (including boron nitride, aluminum nitride, and diamond) were added to a dynamic mixer, heated to 120°C, stirred evenly, and vacuum-stirred for 2 hours. The temperature was lowered to 50°C, 0.22 parts of hydrogen-containing silicone oil and 0.05 parts of inhibitor were added, and vacuum-stirred for 2 hours. 0.2 parts of catalyst were added, and vacuum-stirred for 2 hours. Finally, the product was dispensed.
[0068] Example 8 In the preparation of hyperbranched phenyl vinyl polysiloxane, step (3) is changed to: passing nitrogen containing 50 ppm (volume fraction) oxygen, and the remaining steps and raw material amounts are exactly the same as in Example 7.
[0069] Example 9 The preparation of hyperbranched phenyl vinyl polysiloxane is carried out according to steps (1) and (2) of Example 1.
[0070] Before step (3), the vinyl-terminated polysiloxane raw material obtained in step (2) is adjusted to control its water content at 30 ppm.
[0071] (3) Preparation of hyperbranched phenyl vinyl polysiloxane First, 50g of the prepared hydrogen-containing polysiloxane and 2ppm of platinum catalyst were added to a dry reaction flask, high-purity nitrogen gas was introduced, and the temperature was raised to 90℃. Then, 45g of the terminal vinylphenyl polysiloxane containing 30ppm of water was slowly added dropwise to the reaction flask over a period of 1 hour. The mixture was kept at 90℃ and stirred for 15 hours to finally obtain hyperbranched phenyl vinylpolysiloxane.
[0072] (4) The preparation formula and process of the single-component thermal conductive gel are the same as in Example 7.
[0073] Comparative Example 1 (1) First, add 100 g of tetramethylcyclotetrasiloxane (D4H), 100 g of octamethylcyclotetrasiloxane (D4), and 48.6 g of hexamethyldisiloxane (MM) to a dry 1L reaction flask and dry under vacuum at 100°C for 2 hours. Purge with nitrogen, cool to 60°C, and add 2 ppm of tetramethylammonium hydroxide silanolate (alkali gel). Raise the temperature to 120°C and stir for 6 hours. Gradually raise the temperature to 145~155°C and stir to break down the catalyst for 2 hours. Maintain the temperature at 150°C and remove low-boiling substances under vacuum for 2 hours, finally obtaining a side-containing hydrogen polysiloxane with a yield of 96%.
[0074] (2) First, 100 g of methylphenylcyclotetrasiloxane (D4Ph), 28 g of octamethylcyclotetrasiloxane (D4), and 20.1 g of tetramethyldivinyldisiloxane were added to a dry 1L reaction flask and dried under vacuum at 100°C for 2 hours. Nitrogen gas was introduced, and the temperature was lowered to 60°C. Then, 2 ppm of tetramethylammonium hydroxide silanolate (alkali gel) was added. The temperature was raised to 100~120°C, and the reaction was stirred for 6 hours. The temperature was gradually raised to 150°C, and the reaction was stirred to break down the catalyst for 2 hours. The temperature was maintained at 150°C, and low-boiling substances were removed under vacuum for 2 hours to finally obtain terminal vinylphenyl polysiloxane with a yield of 98%.
[0075] (3) First, add 50 g of the prepared hydrogen-containing polysiloxane and 2 ppm of platinum catalyst to a dry reaction flask, purge with nitrogen, and heat to 90°C. Slowly add 45 g of end-terminated vinylphenyl polysiloxane to the reaction flask over 1 hour. Maintain the temperature at 60°C and stir for 15 hours to finally obtain hyperbranched phenyl vinylpolysiloxane with a yield of 95%.
[0076] (4) Add 2 parts of hyperbranched phenyl vinyl polysiloxane, 1.5 parts of methyl silicone oil, 2 parts of vinyl silicone oil, 0.2 parts of additives, and 96 parts of thermally conductive fillers (including boron nitride, aluminum nitride, and diamond) to a dynamic mixer, heat to 120°C, stir evenly, and vacuum stir for 2 hours. Cool to 50°C, add 0.24 parts of hydrogen-containing silicone oil and 0.05 parts of inhibitor, and vacuum stir for 2 hours. Add 0.2 parts of catalyst, vacuum stir for 2 hours, and finally dispense the material.
[0077] Comparative Example 2 (1) First, add 100 g of tetramethylcyclotetrasiloxane (D4H), 100 g of octamethylcyclotetrasiloxane (D4), and 48.6 g of hexamethyldisiloxane (MM) to a dry 1L reaction flask and dry under vacuum at 100°C for 2 hours. Purge with nitrogen, cool to 60°C, and add 2 ppm of tetramethylammonium hydroxide silanolate (alkali gel). Raise the temperature to 120°C and stir for 6 hours. Gradually raise the temperature to 145~155°C and stir to break down the catalyst for 2 hours. Maintain the temperature at 150°C and remove low-boiling substances under vacuum for 2 hours, finally obtaining a side-containing hydrogen polysiloxane with a yield of 96%.
[0078] (2) First, 100 g of methylphenylcyclotetrasiloxane (D4Ph), 28 g of octamethylcyclotetrasiloxane (D4), and 20.1 g of tetramethyldivinyldisiloxane were added to a dry 1L reaction flask and dried under vacuum at 100°C for 2 hours. Nitrogen gas was introduced, and the temperature was lowered to 60°C. Then, 2 ppm of tetramethylammonium hydroxide silanolate (alkali gel) was added. The temperature was raised to 100~120°C, and the reaction was stirred for 6 hours. The temperature was gradually raised to 150°C, and the reaction was stirred to break down the catalyst for 2 hours. The temperature was maintained at 150°C, and low-boiling substances were removed under vacuum for 2 hours to finally obtain terminal vinylphenyl polysiloxane with a yield of 98%.
[0079] (3) First, add 50 g of the prepared hydrogen-containing polysiloxane and 2 ppm of platinum catalyst to a dry reaction flask, purge with nitrogen, and heat to 90°C. Slowly add 45 g of end-terminated vinylphenyl polysiloxane to the reaction flask over 1 hour. Maintain the temperature at 60°C and stir for 15 hours to finally obtain hyperbranched phenyl vinylpolysiloxane with a yield of 95%.
[0080] (4) Add 1 part of hyperbranched phenyl vinyl polysiloxane, 1.5 parts of methyl silicone oil, 3 parts of vinyl silicone oil, 0.2 parts of additives, and 96 parts of thermally conductive fillers (including boron nitride, aluminum nitride, and diamond) to a dynamic mixer, heat to 120°C, stir evenly, and vacuum stir for 2 hours. Cool to 50°C, add 0.26 parts of hydrogen-containing silicone oil and 0.05 parts of inhibitor, and vacuum stir for 2 hours. Add 0.2 parts of catalyst, vacuum stir for 2 hours, and finally dispense the material.
[0081] Comparative Example 3 (1) First, add 100 g of tetramethylcyclotetrasiloxane (D4H), 100 g of octamethylcyclotetrasiloxane (D4), and 48.6 g of hexamethyldisiloxane (MM) to a dry 1L reaction flask and dry under vacuum at 100°C for 2 hours. Purge with nitrogen, cool to 60°C, and add 2 ppm of tetramethylammonium hydroxide silanolate (alkali gel). Raise the temperature to 120°C and stir for 6 hours. Gradually raise the temperature to 145~155°C and stir to break down the catalyst for 2 hours. Maintain the temperature at 150°C and remove low-boiling substances under vacuum for 2 hours, finally obtaining a side-containing hydrogen polysiloxane with a yield of 96%.
[0082] (2) First, 100 g of methylphenylcyclotetrasiloxane (D4Ph), 28 g of octamethylcyclotetrasiloxane (D4), and 20.1 g of tetramethyldivinyldisiloxane were added to a dry 1L reaction flask and dried under vacuum at 100°C for 2 hours. Nitrogen gas was introduced, and the temperature was lowered to 60°C. Then, 2 ppm of tetramethylammonium hydroxide silanolate (alkali gel) was added. The temperature was raised to 100~120°C, and the reaction was stirred for 6 hours. The temperature was gradually raised to 150°C, and the reaction was stirred to break down the catalyst for 2 hours. The temperature was maintained at 150°C, and low-boiling substances were removed under vacuum for 2 hours to finally obtain terminal vinylphenyl polysiloxane with a yield of 98%.
[0083] (3) First, add 50 g of the prepared hydrogen-containing polysiloxane and 2 ppm of platinum catalyst to a dry reaction flask, purge with nitrogen, and heat to 90°C. Slowly add 45 g of end-terminated vinylphenyl polysiloxane to the reaction flask over 1 hour. Maintain the temperature at 60°C and stir for 15 hours to finally obtain hyperbranched phenyl vinylpolysiloxane with a yield of 95%.
[0084] (4) Add 1.5 parts of methyl silicone oil, 4 parts of vinyl silicone oil, 0.2 parts of additives, and 96 parts of thermally conductive fillers (including boron nitride, aluminum nitride, and diamond) to a dynamic mixer, heat to 120°C, stir evenly, and vacuum stir for 2 hours. Cool to 50°C, add 0.26 parts of hydrogen-containing silicone oil and 0.05 parts of inhibitor, and vacuum stir for 2 hours. Add 0.2 parts of catalyst, vacuum stir for 2 hours, and finally dispense the material.
[0085] Comparative Example 4 In the preparation of hyperbranched phenyl vinyl polysiloxane, step (3) is changed to: passing nitrogen containing 200 ppm (volume fraction) oxygen, and the remaining steps and raw material amounts are exactly the same as in Example 7.
[0086] The preparation formula and process of the single-component thermally conductive gel are the same as in Example 7.
[0087] Comparative Example 5 In the preparation of hyperbranched phenyl vinyl polysiloxane, before step (3), the water content of the terminal vinyl phenyl polysiloxane raw material is adjusted to 100 ppm, and the remaining steps and raw material usage are exactly the same as in Example 9.
[0088] The preparation formula and process of the single-component thermally conductive gel are the same as in Example 7.
[0089] Table 1 The overall data trend analysis in the table above shows that the technical solution of this invention successfully achieved its design goals. In Examples 1 to 6, by using a self-made hyperbranched phenylvinyl polysiloxane combined with a high proportion (80-97 parts) of thermally conductive filler, the prepared gels achieved a wide range of high thermal conductivity (8.06 to 20.05 W / (m·K)) while maintaining excellent high resilience (89.5% to 98.0%) and good heat resistance (initial decomposition temperature all above 210℃). This indicates that the self-made polymer effectively reconciled the contradiction between thermal conductivity, resilience, and heat resistance in a highly filled system.
[0090] The data from Comparative Examples 1 to 3 provide crucial comparative evidence. When the self-made hyperbranched polymer was gradually reduced or even completely eliminated (Comparative Examples 1-3), even though the thermal conductivity remained at a high level (approximately 15 W / (m·K)), the material's resilience deteriorated sharply (from 76.3% to 19.1%), and the heat resistance temperature also decreased significantly (from 195℃ to 152℃). This directly demonstrates that the self-made polymer with the specific structure described is an indispensable key component for achieving high resilience and high heat resistance, an effect that cannot be achieved through conventional linear silicone oils or simple compounding.
[0091] Of particular note are the data from Examples 7 through 9, which validate the unexpected technical effects of introducing the "controlled trace oxygen / water" feature in the hyperbranching polymerization step. Compared to the performance of Example 4 (strictly anhydrous and oxygen-free conditions, serving as the process baseline), Examples 7 (introducing 20 ppm O2) and 9 (introducing 30 ppm H2O) further improved the resilience to 98.9% and 99.3% while maintaining similarly high thermal conductivity and hardness, and simultaneously increased the initial decomposition temperatures to 225°C and 228°C, respectively. This indicates that the controlled trace oxygen or water optimizes the reaction and improves the polymer's fine structure, thereby synergistically enhancing the core performance of the final product. Comparative Examples 4 and 5, however, show that when the oxygen or water content exceeds the "controlled trace" range (200 ppm O2 or 100 ppm H2O), performance significantly decreases, with both resilience and heat resistance temperatures lower than the baseline Example 1.
[0092] In summary, the data in the table fully demonstrates that this invention, through the design of specific structural polymers and a controlled synthesis process, provides an effective solution that simultaneously endows thermally conductive gels with high thermal conductivity, high resilience, and excellent heat resistance. Its technical effects exceed general expectations in the art. The above embodiments are merely examples; those skilled in the art can make other adjustments within the scope of the claims, and these adjustments should also be considered to fall within the protection scope of this invention.
Claims
1. A one-component thermally conductive gel comprising hyperbranched phenylvinyl polysiloxane, characterized in that, It is prepared from raw materials containing the following components: 2-15 parts of hyperbranched phenyl vinyl polysiloxane 0.2-2 parts of hydrogen-containing silicone oil, Catalyst 0.1~2 parts, Inhibitor 0.05~0.5 parts, 80-97 parts of thermally conductive filler; of which, The hyperbranched phenyl vinyl polysiloxane is prepared by hydrosilylation reaction of side-hydrogen-containing polysiloxane and terminal vinyl phenyl polysiloxane.
2. The single-component thermally conductive gel according to claim 1, characterized in that, The structure of the self-made hyperbranched phenyl vinyl polysiloxane is shown in formula (1): Equation (1); Where a,b,n,m=5~70, and the viscosity is 50~1000 mPa·s.
3. The single-component thermally conductive gel according to claim 1 or 2, characterized in that, The preparation method of the self-made hyperbranched phenyl vinyl polysiloxane includes the following steps: (1) Tetramethylcyclotetrasiloxane, octamethylcyclotetrasiloxane and hexamethyldisiloxane are subjected to ring-opening polymerization reaction under the action of alkaline catalyst to prepare side-hydrogen-containing polysiloxane; (2) Methylphenylcyclotetrasiloxane, octamethylcyclotetrasiloxane and tetramethyldivinyldisiloxane are subjected to ring-opening polymerization reaction under the action of alkaline catalyst to prepare end vinylphenyl polysiloxane. (3) In the presence of a platinum catalyst, the side-hydrogenated polysiloxane obtained in step (1) and the terminal vinylphenyl polysiloxane obtained in step (2) are subjected to a hydrosilylation reaction to obtain the hyperbranched phenyl vinylpolysiloxane.
4. The single-component thermally conductive gel according to claim 2, characterized in that, In step (1), the molar ratio of tetramethylcyclotetrasiloxane, octamethylcyclotetrasiloxane and hexamethyldisiloxane is 1~2:1~2:0.01~0.
04.
5. The single-component thermally conductive gel according to claim 2, characterized in that, In step (2), the molar ratio of methylphenylcyclotetrasiloxane, octamethylcyclotetrasiloxane and tetramethyldivinyldisiloxane is 1~2:0.5~1:0.01~0.
04.
6. The single-component thermally conductive gel according to claim 2, characterized in that, In step (3), the molar ratio of the side-hydrogenated polysiloxane to the end-vinylphenyl polysiloxane is 1~2:1~1.
5.
7. The single-component thermally conductive gel according to claim 1 or 2, characterized in that, The raw materials also include methyl silicone oil and / or vinyl silicone oil; and The amount of methyl silicone oil used is 0-20 parts by weight, and the amount of vinyl silicone oil used is 0-30 parts.
8. The single-component thermally conductive gel according to claim 6, characterized in that, The structure of the methyl silicone oil is shown in formula (2): Equation (2); Where n = 0~8000, and viscosity is 50~1000000 mPa·s.
9. The single-component thermally conductive gel according to claim 6, characterized in that, The structure of the vinyl silicone oil is shown in (2): Equation (3); Where n = 0~8000, and viscosity is 50~1000000 mPa·s.
10. A method for preparing a single-component thermally conductive gel according to any one of claims 1-9, characterized in that, Includes the following steps: The self-made hyperbranched phenyl vinyl polysiloxane and thermally conductive filler are mixed and vacuum stirred at 100~130℃; after cooling to 40~60℃, the hydrogen-containing silicone oil and inhibitor are added and vacuum stirred; finally, the catalyst is added, and the mixture is vacuum stirred before being discharged.