A silicone adhesive, its preparation method and application

By combining modified fillers and crosslinking agents, the problems of long curing time and poor performance compatibility of silicone adhesives are solved, enabling the application of fast-curing and high-performance adhesives suitable for insulating protective layers in the electronics and electrical appliance industries.

CN118725814BActive Publication Date: 2026-06-05GUANGZHOU JOINTAS CHEM +1

Patent Information

Authority / Receiving Office
CN · China
Patent Type
Patents(China)
Current Assignee / Owner
GUANGZHOU JOINTAS CHEM
Filing Date
2024-07-15
Publication Date
2026-06-05

AI Technical Summary

Technical Problem

Existing silicone adhesives have excessively long curing times and are difficult to combine insulation, flame retardancy, and thermal conductivity, resulting in incomplete curing of electronic components before assembly, which poses safety hazards. Furthermore, the insulation performance decreases after adding flame retardant and thermally conductive fillers.

Method used

Modified fillers and crosslinking agents with specific structures are used to form macromolecular crosslinking agents through reaction in an inert atmosphere. These agents are then mixed with polydimethylsiloxane under vacuum conditions, and a catalyst is added to shorten the curing time and improve insulation and adhesion properties.

Benefits of technology

It enables rapid curing of silicone adhesives in a short time, providing high insulation, flame retardancy, and thermal conductivity, meeting the rapid assembly needs of the electronics and electrical appliance industry, reducing costs, and facilitating automated dispensing.

✦ Generated by Eureka AI based on patent content.

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Patent Text Reader

Abstract

The present disclosure provides a silicone adhesive, a preparation method and application thereof, and belongs to the technical field of adhesives. The present disclosure adds modified fillers and specific cross-linking agents, which interact with each other, shortens the curing time of the silicone adhesive, and improves the curing depth, insulation performance and bonding performance of the silicone adhesive on the basis of maintaining the flame retardance and thermal conductivity of the silicone adhesive.
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Description

Technical Field

[0001] This disclosure relates to the field of adhesive technology, specifically to an organosilicon adhesive, its preparation method, and its application. Background Technology

[0002] Single-component room temperature vulcanizing (room temperature vulcanizing) silicone rubber possesses excellent adhesive and mechanical properties, low cost, and ease of automated dispensing. Its outstanding high and low temperature resistance, electrical insulation, and weather resistance make it widely used in construction, electronics, and industrial fields. In particular, dealcoholized room temperature vulcanizing silicone rubber, due to the release of small-molecule alcohols, has a relatively low odor and minimal corrosiveness to electronic components, making it highly favored in the electronics industry. Meanwhile, with increasing demand, the electronics industry has higher requirements for workability and safety, including properties such as insulation, flame retardancy, and thermal conductivity. Currently, when using room temperature vulcanizing silicone rubber as an insulating protective layer for electronic components, it is necessary to wait for the silicone adhesive to fully cure (≥7 days) to achieve the required insulation protection function. However, due to production schedules, assembly often occurs before the adhesive has cured. The enclosed environment hinders the curing of the silicone adhesive, thus posing a safety hazard to electronic components. In addition, by adding a large amount of flame-retardant and thermally conductive fillers to silicone adhesives to meet the requirements of flame retardancy and thermal conductivity, however, flame-retardant and thermally conductive fillers contain a lot of metal ions. The greater the amount added, the higher the concentration of metal ions in the silicone adhesive, which easily forms conductive channels, leading to a decrease in the insulation performance of the silicone adhesive.

[0003] Therefore, there is an urgent need to develop an organosilicon adhesive that has a short curing time and combines insulation, flame retardancy, and thermal conductivity. Summary of the Invention

[0004] The purpose of this invention is to overcome the shortcomings of the prior art and provide an organosilicon adhesive with short curing time, insulation, flame retardancy and thermal conductivity, as well as its preparation method and application.

[0005] To achieve the above objectives, the technical solution adopted by the present invention is as follows: In a first aspect, an organosilicon adhesive is provided, comprising the following components in parts by weight: 100 parts of polydimethylsiloxane, 150-500 parts of modified filler, 5-20 parts of crosslinking agent, and 0.1-15 parts of catalyst; wherein the crosslinking agent has the structural formula shown in Formula I:

[0006]

[0007] In Formula I, n = 1-10, R1 is methyl or ethyl, and R2, R3, R4, R5, and R6 are each independently selected from methyl, phenyl, vinyl, aminopropyl, methoxy, ethoxy, alkoxy containing epoxy group, and alkyl containing acrylate group;

[0008] The modified filler includes a first filler and a surface treatment agent, wherein the surface treatment agent is at least one of n-butoxymethacrylamide and tris(trimethoxysilylpropyl)polyisocyanate.

[0009] In some embodiments, the crosslinking agent is prepared by reacting organosilicon monomers and pure water at a temperature of -10 to 40°C for 20 to 60 minutes in an inert atmosphere, and then reacting them at a temperature of 100 to 150°C and a vacuum of (-0.097) to (-0.092) MPa for 30 to 90 minutes to obtain the crosslinking agent.

[0010] In some embodiments, the organosilicon monomer is at least one selected from vinyltrimethoxysilane, vinyltriethoxysilane, methyltrimethoxysilane, methyltriethoxysilane, tetramethoxysilane, phenyltrimethoxysilane, γ-aminopropyltriethoxysilane, γ-aminopropyltrimethoxysilane, 3-aminopropylmethyldimethoxysilane, 3-aminopropylmethyldiethoxysilane, 3-(methacryloyloxy)propyltrimethoxysilane, and γ-[(2,3)-epoxypropyl]propyltrimethoxysilane.

[0011] In some embodiments, the mass of the purified water is 0.1-5 wt% of the mass of the organosilicon monomer.

[0012] In some embodiments, the surface treatment agent further includes at least one of a silane coupling agent and a polyvinylpyrrolidone.

[0013] In some embodiments, the modified filler is prepared by mixing and stirring the first filler and the surface treatment agent at a temperature of 80-120°C for 1-3 hours, and then reacting them at a temperature of 100-150°C and a vacuum degree of <-0.092MPa for 2-4 hours to obtain the modified filler; wherein the mass of the surface treatment agent is 0.5-5wt% of the mass of the first filler.

[0014] In some embodiments, the polydimethylsiloxane is at least one of α,ω-dihydroxy polydimethylsiloxane, methyldimethoxy-terminated polydimethylsiloxane, trimethoxy-terminated polydimethylsiloxane, and vinyldimethoxy-terminated polydimethylsiloxane.

[0015] In some embodiments, the polydimethylsiloxane has a dynamic viscosity of 750-20000 mPa·s at 25°C.

[0016] In some embodiments, the catalyst is at least one of dioctyltin diacetate, dioctyltin dilaurate, dioctyltin dioctate, dibutyltin diacetate, dibutyltin dilaurate, dibutyltin dioctate, isopropyl titanate, n-butyl titanate, ethyl acetoacetate chelate of isopropyl titanate, and acetylacetone chelate of isopropyl titanate.

[0017] In some embodiments, the filler is at least one selected from calcium carbonate, zinc borate, titanium dioxide, silica powder, quartz powder, aluminum hydroxide, alumina, silica, carbon black, magnesium oxide, zinc oxide, magnesium hydroxide, nitrogen-based flame retardants, and phosphorus-based flame retardants.

[0018] Secondly, a method for preparing the aforementioned silicone adhesive is provided, comprising the following steps:

[0019] Polydimethylsiloxane and modified filler were dehydrated at 100-150℃ and under a vacuum of (-0.097)-(-0.092) MPa for 2-4 hours, then cooled to below 40℃, and crosslinking agent and catalyst were added. The mixture was stirred and reacted for 20-40 minutes to obtain silicone adhesive.

[0020] Thirdly, an elastomer is provided, which is obtained by cross-linking and hardening the silicone adhesive.

[0021] Fourthly, the application of the aforementioned silicone adhesive in the preparation of an insulating protective layer is provided.

[0022] Compared with the prior art, the beneficial effects of the present invention are as follows: By adding modified fillers and crosslinking agents of Formula I, the two interact to shorten the curing time of silicone adhesives while maintaining their flame retardant and thermal conductivity properties, and improve their curing depth, insulation properties, and adhesive properties. The silicone adhesive of the present invention can cure rapidly at a temperature of 23±2℃ and a humidity of 50±5%, and has high flame retardancy, thermal conductivity, adhesion, and insulation properties, meeting the needs of rapid assembly in the electronics and electrical appliance industry. It is also low in cost and easy to automate dispensing. Detailed Implementation

[0023] To facilitate understanding of this disclosure, a more complete description will be provided below. However, this disclosure may be implemented in many different forms and is not limited to the embodiments described herein. Rather, these embodiments are provided to provide a more thorough and complete understanding of the disclosure.

[0024] As used in this article:

[0025] "Prepared from" is synonymous with "comprising". The terms "comprising", "including", "having", "containing", or any other variations thereof as used herein are intended to cover non-exclusive inclusion. For example, a composition, step, method, article, or apparatus that includes the listed elements is not necessarily limited to those elements, but may include other elements not expressly listed or elements inherent to such composition, step, method, article, or apparatus.

[0026] The conjunction "composed of..." excludes any unspecified elements, steps, or components. If used in a claim, this phrase makes the claim closed, excluding materials other than those described, except for associated conventional impurities. When the phrase "composed of..." appears in a clause of the body of a claim rather than immediately following it, it limits only the elements described in that clause; other elements are not excluded from the claim as a whole.

[0027] When a quantity, concentration, or other value or parameter is expressed as a range, a preferred range, or a range defined by a series of upper and lower preferred values, this should be understood as specifically disclosing all ranges formed by any pair of any upper or preferred value with any lower or preferred value, regardless of whether the range is disclosed individually. For example, when the range “1-5” is disclosed, the described range should be interpreted as including ranges “1-4”, “1-3”, “1-2”, “1-2 and 4-5”, “1-3 and 5”, etc. When numerical ranges are described herein, unless otherwise stated, the range is intended to include its endpoints and all integers and fractions within that range.

[0028] In these embodiments, unless otherwise specified, the portions and percentages are all by weight.

[0029] "Parts by mass" refers to the basic unit of measurement that expresses the mass ratio of multiple components. One part can represent any unit mass, such as 1g or 2.689g. If we say that component A has "a" parts by mass and component B has "b" parts by mass, it means the ratio of the mass of component A to the mass of component B is a:b. Alternatively, it can mean that the mass of component A is aK and the mass of component B is bK (K is any number representing a multiplier). It is important to understand that, unlike the number of parts by mass, the sum of the mass parts of all components is not limited to 100 parts.

[0030] "And / or" is used to indicate that one or both of the described situations may occur, for example, A and / or B includes (A and B) and (A or B).

[0031] To address the problems of long curing time and the inability to simultaneously achieve insulation, flame retardancy, and thermal conductivity in existing silicone adhesives.

[0032] A first aspect of this disclosure provides an organosilicon adhesive comprising the following components in parts by weight: 100 parts of polydimethylsiloxane, 150-500 parts of modified filler, 5-20 parts of crosslinking agent, and 0.1-15 parts of catalyst; wherein the crosslinking agent has a structural formula as shown in Formula I:

[0033]

[0034] In Formula I, n = 1-10, R1 is methyl or ethyl, and R2, R3, R4, R5, and R6 are each independently selected from methyl, phenyl, vinyl, aminopropyl, methoxy, ethoxy, alkoxy containing epoxy group, and alkyl containing acrylate group;

[0035] The modified filler includes a first filler and a surface treatment agent, wherein the surface treatment agent is at least one of n-butoxymethacrylamide and tris(trimethoxysilylpropyl)polyisocyanate.

[0036] This disclosure, by adding modified fillers and crosslinking agents of Formula I, achieves a combination of the two, which, while maintaining the flame retardant and thermal conductivity properties of silicone adhesives, shortens the curing time and improves the curing depth, insulation properties, and adhesive properties of silicone adhesives.

[0037] In this process, at least one of n-butoxymethacrylamide and tris(trimethoxysilylpropyl)polyisocyanate is used as the first surface treatment agent. The first surface treatment agent is used to treat the surface of the first filler, which reduces the mobility of free metal ions in the silicone adhesive, thereby disrupting the formation of conductive channels in the silicone adhesive and improving the insulation of the silicone adhesive. In addition, the polar groups such as amino, epoxy or carbonyl groups in the crosslinking agent of Formula I complex and modify the metal ions in the filler, restricting the formation of conductive channels by metal ions in the silicone adhesive and improving the insulation of the silicone adhesive.

[0038] The active alkoxy groups in the crosslinking agent react with water vapor in the air, releasing small alcohol molecules to form silanol intermediates. The hydroxyl groups in the resulting silanol intermediates react with the hydroxyl or alkoxy groups in polydimethylsiloxane to form a crosslinked network system, i.e., silicone rubber. Because the crosslinking agent is formed through a pre-hydrolysis reaction, it is a relatively large molecule. The reaction between these large molecules is highly reactive, allowing for rapid curing even in the presence of small amounts of water vapor. This achieves rapid and deep curing, shortens curing time, reduces sensitivity to water vapor content, and enhances the ability to restrict metal ion activity, thereby improving the insulation properties of the silicone adhesive. Compared to small-molecule silane coupling agents, the crosslinking agent of this invention contains a large number of polar groups, such as amino, epoxy, or carbonyl groups. With the same contact area with the substrate, the silicone adhesive has a greater number and variety of polar groups participating in the interaction between the silicone adhesive and the substrate, resulting in better adhesion performance and wider adhesion range.

[0039] Specifically, examples of the epoxy-containing alkoxy group can be...

[0040] Specifically, an example of the alkyl group containing an acrylate group can be —(CH2)3OOC(CH3)C=CH2;

[0041] Specifically, the modified filler may be, but is not limited to, 150 parts, 170 parts, 200 parts, 230 parts, 250 parts, 300 parts, 350 parts, 400 parts, 420 parts, 450 parts, 480 parts, or 500 parts by weight.

[0042] Specifically, the weight parts of the crosslinking agent can be, but are not limited to, 5 parts, 7 parts, 10 parts, 12 parts, 15 parts, 17 parts, or 20 parts.

[0043] Specifically, the catalyst may be, but is not limited to, 0.1 parts, 0.5 parts, 1 part, 3 parts, 5 parts, 7 parts, 9 parts, 11 parts, 13 parts, or 15 parts by weight.

[0044] In one embodiment, the surface treatment agent is n-butoxymethacrylamide and tris(trimethoxysilylpropyl)polyisocyanate, wherein the mass ratio of n-butoxymethacrylamide to tris(trimethoxysilylpropyl)polyisocyanate is 4:1 to 1:6, for example, but not limited to 4:1, 3:1, 2:1, 1:1, 1:2, 1:3, 1:4, 1:5, 1:6, preferably 3:1 to 1:3.

[0045] When the mass ratio of n-butoxymethacrylamide to tris(trimethoxysilylpropyl)polyisocyanate is within the above range, the resulting silicone adhesive has higher curing depth, insulation properties, and bonding properties.

[0046] In some embodiments, the crosslinking agent is prepared by reacting organosilicon monomers and pure water at a temperature of -10 to 40°C for 20 to 60 minutes in an inert atmosphere, and then reacting them at a temperature of 100 to 150°C and a vacuum of (-0.097) to (-0.092) MPa for 30 to 90 minutes to obtain the crosslinking agent.

[0047] In some embodiments, the organosilicon monomer is at least one selected from vinyltrimethoxysilane, vinyltriethoxysilane, methyltrimethoxysilane, methyltriethoxysilane, tetramethoxysilane, phenyltrimethoxysilane, γ-aminopropyltriethoxysilane, γ-aminopropyltrimethoxysilane, 3-aminopropylmethyldimethoxysilane, 3-aminopropylmethyldiethoxysilane, 3-(methacryloyloxy)propyltrimethoxysilane, and γ-[(2,3)-epoxypropyl]propyltrimethoxysilane.

[0048] The crosslinking agent disclosed herein is a hydrolysis product of organosilicon monomers. After hydrolysis, the organosilicon monomers form macromolecules through condensation reactions between Si-OH groups, which improves the reactivity of the crosslinking agent. In the presence of a small amount of water vapor, it can react rapidly with polydimethylsiloxane, shortening the curing time of the silicone adhesive and reducing the sensitivity to low water content. This limits the activity of metal ions in the silicone adhesive and improves its insulation. In addition, the crosslinking agent self-crosslinks to form a three-dimensional Si-O-Si network structure. The crosslinking network structure formed by the crosslinking agent and polydimethylsiloxane is intertwined and connected to the substrate through strong chemical bonds during the curing process, thereby improving the bonding strength of the silicone adhesive.

[0049] In some embodiments, the mass of the purified water is 0.1-5 wt% of the mass of the organosilicon monomer, for example, but not limited to 0.1 wt%, 0.3 wt%, 0.5 wt%, 0.7 wt%, 1 wt%, 1.5 wt%, 2 wt%, 2.5 wt%, 3 wt%, 3.5 wt%, 4 wt%, 4.2 wt%, 4.5 wt%, 4.8 wt%, and 5 wt%.

[0050] In some embodiments, the surface treatment agent further includes at least one of a silane coupling agent and a polyvinylpyrrolidone.

[0051] This disclosure uses at least one of silane coupling agent and polyvinylpyrrolidone as a second surface treatment agent. By adding the second surface treatment agent on the basis of the first surface treatment agent, the modification effect of the surface treatment agent on the first filler can be further improved, thereby improving the insulation performance and curing depth of the silicone adhesive.

[0052] Specifically, the silane coupling agent is at least one of bis(N-methylbenzamide)ethoxymethylsilane, 3-ureapropyltrimethoxysilane, N-(piperazinylethyl)-3-aminopropylmethyldimethoxysilane, 3-piperazinylpropylmethyldimethoxysilane, and polyethylene glycol trimethoxysilyl ether.

[0053] Specifically, the mass ratio of the first surface treatment agent to the second surface treatment agent is 6:1 to 1:2, for example, but not limited to 6:1, 5:1, 4:1, 3:1, 2:1, 1:1, and 1:2.

[0054] In some embodiments, the modified filler is prepared by mixing and stirring the first filler and the surface treatment agent at a temperature of 80-120°C for 1-3 hours, and then reacting them at a temperature of 100-150°C and a vacuum degree of <-0.092MPa for 2-4 hours to obtain the modified filler.

[0055] Specifically, the surface treatment agent is 0.5-5 wt% of the mass of the first filler, for example, but not limited to 0.5 wt%, 0.8 wt%, 1 wt%, 1.2 wt%, 1.5 wt%, 1.8 wt%, 2 wt%, 2.5 wt%, 3 wt%, 3.5 wt%, 3.7 wt%, 4 wt%, 4.3 wt%, 4.5 wt%, 4.7 wt%, and 5 wt%.

[0056] This disclosure achieves different degrees of modification of the filler by controlling various parameters in the preparation process of the modified filler, such as temperature, time, vacuum degree and the amount of surface treatment agent added, so as to improve the insulation and bonding strength of the silicone adhesive.

[0057] If the mass of the surface treatment agent is less than 0.5 wt% of the mass of the first filler, the modification effect of the filler is poor, and it cannot reduce the activity of free metal ions in the filler, thus reducing the insulation of the silicone adhesive. If the mass of the surface treatment agent is greater than 5 wt% of the mass of the first filler, too much surfactant will coat the filler, making it difficult for it to exert its flame retardant and / or thermal conductivity effects, thus reducing the thermal conductivity and flame retardancy of the silicone adhesive.

[0058] In some embodiments, the polydimethylsiloxane is at least one of α,ω-dihydroxy polydimethylsiloxane, methyldimethoxy-terminated polydimethylsiloxane, trimethoxy-terminated polydimethylsiloxane, and vinyldimethoxy-terminated polydimethylsiloxane.

[0059] In some embodiments, the dynamic viscosity of the polydimethylsiloxane at 25°C is 750-20000 mPa·s, for example, but not limited to 750 mPa·s, 1000 mPa·s, 2000 mPa·s, 5000 mPa·s, 8000 mPa·s, 10000 mPa·s, 12000 mPa·s, 15000 mPa·s, 18000 mPa·s, and 20000 mPa·s.

[0060] In some embodiments, the catalyst is at least one of dioctyltin diacetate, dioctyltin dilaurate, dioctyltin dioctanoate, dibutyltin diacetate, dibutyltin dilaurate, dibutyltin dioctanoate, isopropyl titanate, n-butyl titanate, ethyl acetoacetate chelate of isopropyl titanate, and acetylacetone chelate of isopropyl titanate.

[0061] In some embodiments, the first filler is at least one of thermally conductive filler and flame-retardant filler.

[0062] Thermally conductive fillers are fillers that have a thermal conductivity of at least 5 W / m·K at 25°C (measured according to ASTM D7984). Thermally conductive fillers may comprise particles of a single type of filler material or particles of two or more types of filler materials. That is, a thermally conductive filler may include particles of a first type of thermally conductive filler, and may also include particles of at least a second type of thermally conductive filler, different from the first type. As used herein, the terms "first type" and "second type" regarding filler material types are for convenience only and do not indicate the order of addition.

[0063] Non-limiting examples of thermally conductive fillers include nitrides, metal oxides, quasi-metal oxides, metal hydroxides, arsenides, carbides, minerals, ceramics, and diamond. For example, thermally conductive filler materials may include, consist essentially of, or be composed of the following materials: boron nitride, silicon nitride, aluminum nitride, boron arsenide, aluminum oxide, magnesium oxide, reburned magnesium oxide, beryllium oxide, silicon dioxide, titanium dioxide, zinc oxide, nickel oxide, copper oxide, tin oxide, aluminum hydroxide (i.e., aluminum hydroxide, aluminum trihydrate), magnesium hydroxide, boron arsenide, silicon carbide, agate, corundum sand, ceramic microspheres, diamond, or any combination thereof.

[0064] Flame retardant fillers are materials that slow down or prevent the spread of fire or reduce its strength. Some of the aforementioned TC materials, such as aluminum hydroxide and magnesium hydroxide, can also be flame retardants. As described in more detail below, flame retardants can include minerals, organic compounds, organophosphorus compounds, or combinations thereof. Suitable examples of minerals include calcium magnesium carbonate, magnesia, various hydrates, red phosphorus, boron compounds such as borates, carbonates such as calcium carbonate and magnesium carbonate, and combinations thereof. Suitable examples of organophosphorus compounds include triphenyl phosphate (TPP), resorcinol bis(diphenyl phosphate) (RDP), bisphenol A diphenyl phosphate (BADP), and tricresyl phosphate (TCP); phosphonates, such as dimethyl methylphosphonate (DMMP); and phosphonates, such as aluminum diethylphosphonate. In an important class of flame retardants, the compound contains both phosphorus and halogens. Such compounds include tris(2,3-dibromopropyl) phosphate (tribromophosphate) and chlorinated organophosphates, such as tris(1,3-dichloro-2-propyl) phosphate (tribromophosphate or TDCPP) and tetra(2-chloroethyl)dichloroisopentyl diphosphate (V6). Suitable examples of organic compounds include carboxylic acids, dicarboxylic acids, melamine, and organic nitrogen compounds. Other suitable flame retardants include ammonium polyphosphate and barium sulfate.

[0065] The first packing material can have any particle shape or geometry. For example, the first packing material can be regular or irregular in shape, and can be spherical, elliptical, cubic, plate-like, needle-like (elongated or fibrous), rod-like, disc-like, prismatic, plate-like, rock-like, etc., its agglomerates, and any combination thereof.

[0066] Specifically, the average particle size of the first filler disclosed herein is 0.01 μm-500 μm, for example, but not limited to 0.01 μm, 1 μm, 5 μm, 10 μm, 50 μm, 100 μm, 150 μm, 200 μm, 250 μm, 300 μm, 400 μm, 450 μm, and 500 μm.

[0067] Suitable methods for measuring the average particle size of the first packing include using instruments such as the Quanta 250FEG SEM or equivalent instruments.

[0068] Secondly, a method for preparing the aforementioned silicone adhesive is provided, comprising the following steps:

[0069] Polydimethylsiloxane and modified filler were dehydrated at 100-150℃ and under a vacuum of (-0.097)-(-0.092) MPa for 2-4 hours, then cooled to below 40℃, and crosslinking agent and catalyst were added. The mixture was stirred and reacted for 20-40 minutes to obtain silicone adhesive.

[0070] The silicone adhesive of the present invention is prepared in a closed reactor equipped with a stirrer under moisture-free conditions. If necessary, a vacuum can be created in the reactor, and the expelled air is subsequently replaced with anhydrous gas such as nitrogen.

[0071] Furthermore, to avoid the influence of moisture in the modified packing material, the modified packing material is also prepared under moisture-free conditions in a closed reactor equipped with a stirrer. If necessary, a vacuum can be created in the reactor, and the expelled air is then replaced with anhydrous gas such as nitrogen.

[0072] Examples of equipment include slow dispersers, paddle mixers, spiral mixers, arm mixers, anchor mixers, planetary mixers, hook mixers, and single-screw or multi-screw extruders.

[0073] Thirdly, an elastomer is provided, which is obtained by crosslinking and curing the silicone adhesive. This elastomer is capable of adhering to various substrates.

[0074] The substrate can be metallic or non-metallic. Metallic substrates include, but are not limited to, tin, steel, cold-rolled 61 steel, hot-rolled steel, zinc-coated steel, zinc compounds, zinc alloys, electro-galvanized steel, hot-dip galvanized steel, galvanized steel, aluminized zinc steel, steel-zinc alloys, stainless steel, zinc-aluminum-magnesium alloy steel, zinc-aluminum alloys, aluminum, aluminum alloys, aluminized steel, aluminized alloy steel, galvanized aluminum alloy steel, magnesium, magnesium alloys, nickel, nickel plating, bronze, tinplate, composite materials, titanium, brass, copper, silver, gold, 3D printing metals, cast or forged metals and alloys, or combinations thereof.

[0075] The substrate may include batteries or battery components. Batteries may be, for example, electric vehicle batteries, and battery assemblies may be electric vehicle battery assemblies. Battery assemblies may include, but are not limited to, battery cells, battery housings, battery modules, battery packs, battery boxes, battery cell housings, battery pack housings, battery covers and trays, thermal management systems, inverters, battery housings, module housings, module racks, battery side panels, battery cell shells, cooling modules, cooling pipes, cooling fins, cooling plates, busbars, battery frames, electrical connectors, metal wires, copper or aluminum conductors or cables, any component of a stationary energy storage system, or any combination thereof.

[0076] Fourthly, this disclosure provides applications of the adhesives described herein; the silicone adhesives of the present invention cure at ambient temperature, particularly at temperatures of 5-35°C and in the presence of moisture. These silicone adhesives can be used in a wide range of applications, such as bonding of electronic components, adhesive bonding in the construction industry, and assembly and bonding of a broad range of materials (metals, plastics such as PVC, PMMA, natural rubber, synthetic rubber, wood, sheets, ceramics, bricks, glass, stone, concrete, masonry components) in the construction industry, as well as in the automotive, home appliance, and electronics industries.

[0077] The raw materials used in the embodiments and comparative examples are described below, but are not limited to these materials:

[0078] The first crosslinking agent was prepared in-house. The preparation method was as follows: in an inert atmosphere, organosilicon monomers and pure water were reacted at 10°C for 30 min, and then reacted at 120°C and a vacuum of -0.095 MPa for 60 min to obtain the first crosslinking agent. The organosilicon monomers were a mixture of methyltrimethoxysilane, γ-aminopropyltriethoxysilane and γ-[(2,3)-epoxypropyl]propyltrimethoxysilane in a mass ratio of 7:2:1, and the mass of pure water was 1% of the mass of organosilicon monomers.

[0079] The second crosslinking agent was prepared in-house. The preparation method was as follows: in an inert atmosphere, organosilicon monomers and purified water were reacted at 40°C for 20 min, and then reacted at 150°C and a vacuum of -0.095 MPa for 30 min to obtain the second crosslinking agent. The organosilicon monomers were a mixture of phenyltrimethoxysilane, tetramethoxysilane and 3-aminopropylmethyldimethoxysilane in a mass ratio of 2:2:1, and the mass of purified water was 0.1% of the mass of the organosilicon monomers.

[0080] The third crosslinking agent was prepared in-house. The preparation method was as follows: in an inert atmosphere, organosilicon monomers and purified water were reacted at -10°C for 60 min, and then reacted at 100°C and a vacuum of -0.095 MPa for 90 min to obtain the third crosslinking agent. The organosilicon monomers were a mixture of methyltrimethoxysilane and 3-(methacryloyloxy)propyltrimethoxysilane in a mass ratio of 5:1, and the mass of purified water was 5% of the mass of the organosilicon monomers.

[0081] The fourth crosslinking agent was prepared in-house. The preparation method was as follows: in an inert atmosphere, organosilicon monomers and pure water were reacted at 10°C for 40 min, and then reacted at 100°C and a vacuum of -0.095 MPa for 90 min to obtain the fourth crosslinking agent. The organosilicon monomers were a mixture of methyltrimethoxysilane, γ-aminopropyltriethoxysilane, γ-[(2,3)-epoxypropyl]propyltrimethoxysilane, and 3-(methacryloyloxy)propyltrimethoxysilane in a mass ratio of 10:2:1:2. The mass of pure water was 3% of the mass of the organosilicon monomers.

[0082] The fifth crosslinking agent is self-made. Its preparation method is as follows: methyltrimethoxysilane, γ-aminopropyltriethoxysilane and γ-[(2,3)-epoxypropyl]propyltrimethoxysilane are mixed evenly in a mass ratio of 7:2:1 to obtain the agent.

[0083] Example 1

[0084] This embodiment provides an organosilicon adhesive comprising the following components in parts by weight: 100 parts of trimethoxy-terminated polydimethylsiloxane, 350 parts of modified filler, 10 parts of first crosslinking agent, and 8 parts of diisopropyl bis(ethyl acetoacetate) titanate.

[0085] The modified filler was prepared in-house. The preparation method was as follows: aluminum hydroxide and aluminum oxide were added to a power mixer at a mass ratio of 2:1. The first surface treatment agent was added at 110°C and stirred in a closed environment for 2 hours. Then, the mixture was reacted at 150°C and a vacuum of -0.095 MPa for 3 hours to obtain the modified filler. The first surface treatment agent was n-butoxymethacrylamide, and the mass of the first surface treatment agent was 2 wt% of the total mass of aluminum hydroxide and aluminum oxide.

[0086] The dynamic viscosity of trimethoxy-terminated polydimethylsiloxane at 25°C is 1500 mPa·s.

[0087] This embodiment also provides a method for preparing silicone adhesive, including the following steps:

[0088] Trimethoxy-terminated polydimethylsiloxane and modified filler were added to a power mixer and dehydrated for 3 hours at 150°C and a vacuum of -0.095 MPa. Then, the temperature was lowered to below 40°C, and the first crosslinking agent and diisopropyl bis(ethyl acetoacetate) titanate were added. The mixture was stirred in a closed container for 30 minutes under a vacuum of -0.095 MPa to obtain the silicone adhesive.

[0089] Example 2

[0090] This embodiment provides an organosilicon adhesive comprising the following components in parts by weight: 100 parts of vinyl dimethoxy-terminated polydimethylsiloxane, 150 parts of modified filler, 5 parts of second crosslinking agent, and 0.1 parts of dibutyltin dilaurate;

[0091] The modified filler was prepared in-house. The preparation method was as follows: silicon micro powder, magnesium hydroxide and zinc oxide were added to a power mixer in a mass ratio of 1:2:1. The first surface treatment agent was added at 120°C and stirred in a closed environment for 1 hour. Then, the mixture was reacted at 160°C and a vacuum of -0.095 MPa for 2 hours to obtain the modified filler. The first surface treatment agent was n-butoxymethacrylamide, and the mass of the first surface treatment agent was 0.5 wt% of the total mass of silicon micro powder, magnesium hydroxide and zinc oxide.

[0092] The dynamic viscosity of vinyl dimethoxy-terminated polydimethylsiloxane at 25°C is 20,000 mPa·s.

[0093] This embodiment also provides a method for preparing silicone adhesive, including the following steps:

[0094] Vinyl dimethoxy-terminated polydimethylsiloxane and modified filler were added to a power mixer and dehydrated for 3 hours at 150°C and a vacuum of -0.095 MPa. Then, the temperature was lowered to below 40°C, and a second crosslinking agent and dibutyltin dilaurate were added. The mixture was stirred in a closed container for 30 minutes under a vacuum of -0.095 MPa to obtain an organosilicon adhesive.

[0095] Example 3

[0096] This embodiment provides an organosilicon adhesive comprising the following components in parts by weight: 100 parts of α,ω-dihydroxypolydimethylsiloxane, 500 parts of modified filler, 20 parts of third crosslinking agent, and 15 parts of diisopropyl di(acetylacetone)titanate.

[0097] The modified filler was prepared in-house. The preparation method was as follows: silica powder, alumina and melamine cyanurate were added to a power mixer in a mass ratio of 1:2:1. The first surface treatment agent was added at 80°C and the mixture was stirred in a closed environment for 3 hours. Then, the mixture was reacted at 110°C and a vacuum of -0.095 MPa for 4 hours to obtain the modified filler. The first surface treatment agent was n-butoxymethacrylamide, and the mass of the first surface treatment agent was 5 wt% of the total mass of silica powder, alumina and melamine cyanurate.

[0098] The dynamic viscosity of α,ω-dihydroxypolydimethylsiloxane at 25°C is 1500 mPa·s.

[0099] This embodiment also provides a method for preparing silicone adhesive, including the following steps:

[0100] α,ω-dihydroxypolydimethylsiloxane and modified filler were added to a power mixer and dehydrated for 4 hours at 100℃ and -0.095MPa. Then, the temperature was lowered to below 40℃, and a third crosslinking agent and diisopropyl di(acetylacetone)titanate were added. The mixture was stirred in a closed container for 30 minutes under a vacuum of -0.095MPa to obtain the silicone adhesive.

[0101] Example 4

[0102] This embodiment provides an organosilicon adhesive comprising the following components in parts by weight: 100 parts of α,ω-dihydroxypolydimethylsiloxane, 300 parts of modified filler, 15 parts of fourth crosslinking agent, 4 parts of dioctyltin dilaurate, and 8 parts of diisopropyl bis(ethyl acetoacetate) titanate.

[0103] The modified filler was prepared in-house. The preparation method was as follows: calcium carbonate, aluminum hydroxide, magnesium oxide, and ammonium polyphosphate were added to a power mixer in a mass ratio of 2:6:1:2. The first surface treatment agent was added at 100°C, and the mixture was stirred in a closed environment for 3 hours. Then, the mixture was reacted at 110°C and a vacuum of -0.095 MPa for 4 hours to obtain the modified filler. The first surface treatment agent was n-butoxymethacrylamide, and the mass of the first surface treatment agent was 3 wt% of the total mass of the flame retardant calcium carbonate, aluminum hydroxide, magnesium oxide, and ammonium polyphosphate.

[0104] The dynamic viscosity of α,ω-dihydroxypolydimethylsiloxane at 25°C is 5000 mPa·s.

[0105] This embodiment also provides a method for preparing silicone adhesive, including the following steps:

[0106] α,ω-dihydroxypolydimethylsiloxane and modified filler were added to a power mixer and dehydrated for 3 hours at 120°C and -0.095 MPa. Then, the mixture was cooled to below 40°C, and a fourth crosslinking agent, dioctyltin dilaurate and diisopropyl bis(ethyl acetoacetate) titanate were added. The mixture was stirred in a closed container for 30 minutes under a vacuum of -0.095 MPa to obtain an organosilicon adhesive.

[0107] Example 5

[0108] This embodiment provides an organosilicon adhesive, which differs from the organosilicon adhesive of Example 1 only in that the first surface treatment agent is different. The first surface treatment agent in this embodiment is tris(trimethoxysilylpropyl)polyisocyanate, and the remaining components and amounts are the same as in Example 1.

[0109] The preparation method of the silicone adhesive in this embodiment is the same as that in Example 1.

[0110] Example 6

[0111] This embodiment provides an organosilicon adhesive, which differs from the organosilicon adhesive of Example 1 only in that the first surface treatment agent is different. The first surface treatment agent in this embodiment is n-butoxymethacrylamide and tris(trimethoxysilylpropyl)polyisocyanate, and the mass ratio of n-butoxymethacrylamide to tris(trimethoxysilylpropyl)polyisocyanate is 4:1. The remaining components and amounts are the same as in Example 1.

[0112] The preparation method of the silicone adhesive in this embodiment is the same as that in Example 1.

[0113] Example 7

[0114] This embodiment provides an organosilicon adhesive, which differs from the organosilicon adhesive of Example 1 only in that the first surface treatment agent is different. The first surface treatment agent in this embodiment is n-butoxymethacrylamide and tris(trimethoxysilylpropyl)polyisocyanate, and the mass ratio of n-butoxymethacrylamide to tris(trimethoxysilylpropyl)polyisocyanate is 3:1. The remaining components and amounts are the same as in Example 1.

[0115] The preparation method of the silicone adhesive in this embodiment is the same as that in Example 1.

[0116] Example 8

[0117] This embodiment provides an organosilicon adhesive, which differs from the organosilicon adhesive of Example 1 only in that the first surface treatment agent is different. The first surface treatment agent in this embodiment is n-butoxymethacrylamide and tris(trimethoxysilylpropyl)polyisocyanate, and the mass ratio of n-butoxymethacrylamide and tris(trimethoxysilylpropyl)polyisocyanate is 1:1. The remaining components and amounts are the same as in Example 1.

[0118] The preparation method of the silicone adhesive in this embodiment is the same as that in Example 1.

[0119] Example 9

[0120] This embodiment provides an organosilicon adhesive, which differs from the organosilicon adhesive of Example 1 only in that the first surface treatment agent is different. The first surface treatment agent in this embodiment is n-butoxymethacrylamide and tris(trimethoxysilylpropyl)polyisocyanate, and the mass ratio of n-butoxymethacrylamide and tris(trimethoxysilylpropyl)polyisocyanate is 1:3. The remaining components and amounts are the same as in Example 1.

[0121] The preparation method of the silicone adhesive in this embodiment is the same as that in Example 1.

[0122] Example 10

[0123] This embodiment provides an organosilicon adhesive, which differs from the organosilicon adhesive of Example 1 only in that the first surface treatment agent is different. The first surface treatment agent in this embodiment is n-butoxymethacrylamide and tris(trimethoxysilylpropyl)polyisocyanate, and the mass ratio of n-butoxymethacrylamide and tris(trimethoxysilylpropyl)polyisocyanate is 1:6. The remaining components and amounts are the same as in Example 1.

[0124] The preparation method of the silicone adhesive in this embodiment is the same as that in Example 1.

[0125] Example 11

[0126] This embodiment provides an organosilicone adhesive, which differs from the organosilicone adhesive of Example 1 only in the preparation method of the modified filler. The preparation method of the modified filler in this embodiment is as follows:

[0127] Aluminum hydroxide and aluminum oxide were added to a power mixer at a mass ratio of 2:1. A first surface treatment agent and a second surface treatment agent were added at 110°C, and the mixture was stirred for 2 hours in a sealed environment. The mixture was then reacted for 3 hours at 150°C and a vacuum of -0.095 MPa to obtain the modified filler. The first surface treatment agent was n-butoxymethacrylamide, and the second surface treatment agent was polyvinylpyrrolidone. The total mass of the first and second surface treatment agents was 3 wt% of the total mass of calcium carbonate, aluminum hydroxide, magnesium oxide, and phosphorus-based flame retardant. The mass ratio of the first and second surface treatment agents was 1:1. The remaining components and their dosages were the same as in Example 1.

[0128] The preparation method of the silicone adhesive in this embodiment is the same as that in Example 1.

[0129] Example 12

[0130] This embodiment provides an organosilicon adhesive, which differs from the organosilicon adhesive of Example 11 only in that the second surface treatment agent is different. In this embodiment, the second surface treatment agent is 3-ureapropyltrimethoxysilane; the remaining components and amounts are the same as in Example 11.

[0131] The preparation method of the silicone adhesive in this embodiment is the same as that in Example 11.

[0132] Example 13

[0133] This embodiment provides an organosilicon adhesive, which differs from the organosilicon adhesive of Example 11 only in that the second surface treatment agent is different. In this embodiment, the second surface treatment agent is polyethylene glycol trimethoxysilylpropyl ether; the remaining components and amounts are the same as in Example 11.

[0134] The preparation method of the silicone adhesive in this embodiment is the same as that in Example 11.

[0135] Example 14

[0136] This embodiment provides an organosilicon adhesive, which differs from the organosilicon adhesive of Example 11 only in that the second surface treatment agent is different. In this embodiment, the second surface treatment agent is N-(piperazinylethyl)-3-aminopropylmethyldimethoxysilane; the remaining components and amounts are the same as in Example 11.

[0137] The preparation method of the silicone adhesive in this embodiment is the same as that in Example 11.

[0138] Example 15

[0139] This embodiment provides an organosilicon adhesive, which differs from the organosilicon adhesive of Example 11 only in that the second surface treatment agent is different. In this embodiment, the second surface treatment agent is γ-aminopropyltriethoxysilane; the remaining components and amounts are the same as in Example 11.

[0140] The preparation method of the silicone adhesive in this embodiment is the same as that in Example 11.

[0141] Example 16

[0142] This embodiment provides an organosilicon adhesive, which differs from the organosilicon adhesive of Example 11 only in that the first surface treatment agent is different. The first surface treatment agent in this embodiment is n-butoxymethacrylamide and tris(trimethoxysilylpropyl)polyisocyanate, and the mass ratio of n-butoxymethacrylamide and tris(trimethoxysilylpropyl)polyisocyanate is 1:1; the remaining components and amounts are the same as in Example 11.

[0143] The preparation method of the silicone adhesive in this embodiment is the same as that in Example 11.

[0144] Comparative Example 1

[0145] This comparative example provides an organosilicon adhesive comprising the following components in parts by weight: 100 parts of trimethoxy-terminated polydimethylsiloxane, 350 parts of filler, 10 parts of fifth crosslinking agent, and 8 parts of diisopropyl bis(ethyl acetoacetate) titanate.

[0146] The filler is a mixture of aluminum hydroxide and aluminum oxide, with a mass ratio of aluminum hydroxide to aluminum oxide of 2:1; the dynamic viscosity of trimethoxy-terminated polydimethylsiloxane at 25°C is 1500 mPa·s.

[0147] This embodiment also provides a method for preparing silicone adhesive, including the following steps:

[0148] Trimethoxy-terminated polydimethylsiloxane and filler were added to a power mixer and dehydrated for 3 hours at 150°C and a vacuum of -0.095 MPa. Then, the temperature was lowered to below 40°C, and a fifth crosslinking agent and diisopropyl bis(ethyl acetoacetate) titanate were added. The mixture was stirred in a closed container for 30 minutes under a vacuum of -0.095 MPa to obtain an organosilicon adhesive.

[0149] Comparative Example 2

[0150] This comparative example provides an organosilicon adhesive that differs from the organosilicon adhesive of Example 1 only in that a fifth crosslinking agent is used instead of the first crosslinking agent, while the remaining components and amounts are the same as in Example 1.

[0151] The preparation method of the comparative silicone adhesive is the same as that of Example 1.

[0152] Comparative Example 3

[0153] This comparative example provides an organosilicone adhesive, which differs from the organosilicone adhesive of Example 1 only in that: a filler is used instead of a modified filler. The filler in this comparative example is a mixture of aluminum hydroxide and aluminum oxide, with a mass ratio of aluminum hydroxide to aluminum oxide of 2:1; the remaining components and amounts are the same as in Example 1.

[0154] The preparation method of the comparative silicone adhesive is the same as that of Example 1.

[0155] Comparative Example 4

[0156] This comparative example provides an organosilicon adhesive that differs from the organosilicon adhesive of Example 1 only in that a second surface treatment agent is used instead of the first surface treatment agent, and the second surface treatment agent is 3-ureapropyltrimethoxysilane; the remaining components and amounts are the same as in Example 1.

[0157] The preparation method of the comparative silicone adhesive is the same as that of Example 1.

[0158] Comparative Example 5

[0159] This comparative example provides an organosilicon adhesive, which differs from the organosilicon adhesive of Example 1 only in that a second surface treatment agent is used instead of the first surface treatment agent, and the second surface treatment agent is polyvinylpyrrolidone; the remaining components and amounts are the same as in Example 1.

[0160] The preparation method of the comparative silicone adhesive is the same as that of Example 1.

[0161] Performance testing

[0162] The properties of the silicone adhesives obtained in the examples and comparative examples were tested, and the specific test methods are as follows:

[0163] (1) Surface drying time: Tested according to GB / T 13477-1992.

[0164] (2) Curing depth: The silicone adhesive was poured into the wedge-shaped groove of the polytetrafluoroethylene test plate with a wedge-shaped groove. The size of the wedge-shaped groove was 5cm×5cm×20cm. Then the test plate was placed under the conditions of 23±2℃ and 50±5% relative humidity to cure and form a test sample. After 4 hours, the test sample was peeled off from the test plate and the curing depth of the silicone adhesive was compared.

[0165] (3) Insulation resistance: Under the conditions of temperature of 23±2℃ and relative humidity of 50±5%, 100g of silicone adhesive was weighed in a disposable plastic cup. The voltage of the insulation resistance meter was set to 1000V, and the range of insulation resistance was 0~19.99GΩ (when it is greater than 19.99, the display is also 19.99). The distance between the positive and negative electrodes was fixed at 5mm. The positive and negative electrodes were inserted into the uncured silicone adhesive at the same time. After the data stabilized, the insulation resistance data was recorded. The insulation resistance meter was purchased from Xi'an Shengli Instrument Co., Ltd., and the model was VICTOR 60H.

[0166] (4) Flame retardant rating: According to UL94 test.

[0167] (5) Thermal conductivity: Tested according to ASTM D5470.

[0168] (6) Volume resistivity: Tested according to GB / T 1692.

[0169] (7) Shear strength: Tested according to GB / T 7124.

[0170] The test results are shown in Table 1.

[0171] Table 1

[0172]

[0173]

[0174] As shown in Table 1, the experimental data of the disclosed silicone adhesive shows that the curing depth after 4 hours is 1.59-2.31 mm, the insulation resistance of the uncured state is 12.26-19.99 GΩ, and the volume resistivity after curing is 1.2 × 10⁻⁶. 12 -8.6×10 16 The shear strength is 1.8-2.9 MPa (Ω·cm). This indicates that the silicone adhesive disclosed herein, while maintaining the flame retardant and thermal conductivity properties of silicone adhesives, shortens the curing time and improves the curing depth, insulation properties, and adhesive properties of silicone adhesives.

[0175] Comparing Examples 1 and 5-10, it can be seen that when the first surface treatment agent is n-butoxymethacrylamide and tris(trimethoxysilylpropyl)polyisocyanate, the resulting silicone adhesive has a curing depth of 1.85-2.31 mm after 4 hours, an insulation resistance of 17.72-19.99 GΩ before curing, and a volume resistivity of 5.3 × 10⁻⁶ after curing. 15 -8.6×10 16 Ω·cm; This indicates that the silicone adhesive disclosed herein has a higher curing depth and insulation properties.

[0176] Comparing Examples 1 and 11-15, it can be seen that when the surface treatment agent is the first surface treatment agent and the second surface treatment agent, the cured silicone adhesive has a curing depth of 1.79-1.91 mm after 4 hours, an insulation resistance of 14.11-16.96 GΩ before curing, and a volume resistivity of 7.3 × 10⁻⁶ after curing. 13 -8.2×10 15 Ω·cm; This indicates that the silicone adhesive disclosed herein has a higher curing depth and insulation properties.

[0177] Comparing Example 1 and Comparative Examples 1-3, it can be seen that if the filler is not modified and / or the crosslinking agent is not within the scope of the present invention, the 4-hour curing depth, uncured insulation resistance, cured volume resistivity, and shear strength of the obtained silicone adhesive are significantly reduced.

[0178] Comparing Example 1 and Comparative Examples 4-5, it can be seen that when only silane coupling agent or polyvinylpyrrolidone is used as a surface treatment agent to modify the filler, the 4-hour curing depth, uncured insulation resistance, cured volume resistivity, and shear strength of the resulting silicone adhesive are significantly reduced.

[0179] Finally, it should be noted that the above embodiments are used to illustrate the technical solutions of the present invention and not to limit the scope of protection of the present invention. Although the present invention has been described in detail with reference to preferred embodiments, those skilled in the art should understand that modifications or equivalent substitutions can be made to the technical solutions of the present invention without departing from the essence and scope of the technical solutions of the present invention.

Claims

1. An organosilicon adhesive, characterized in that, The product comprises the following components in parts by weight: 100 parts polydimethylsiloxane, 150-500 parts modified filler, 5-20 parts crosslinking agent, and 0.1-15 parts catalyst; wherein the crosslinking agent has the structural formula shown in Formula I: Equation I In Formula I, n = 1-10, R1 is methyl or ethyl, and R2, R3, R4, R5, and R6 are each independently selected from methyl, phenyl, vinyl, aminopropyl, methoxy, ethoxy, alkoxy containing epoxy group, and alkyl containing acrylate group. The modified filler includes a first filler and a surface treatment agent, wherein the surface treatment agent is at least one of n-butoxymethacrylamide and tris(trimethoxysilylpropyl)polyisocyanate; The modified filler is prepared by mixing and stirring the first filler and the surface treatment agent at a temperature of 80-120℃ for 1-3 hours, and then reacting at a temperature of 100-150℃ and a vacuum degree of <-0.092MPa for 2-4 hours to obtain the modified filler; wherein, the mass of the surface treatment agent is 0.5-5wt% of the mass of the first filler.

2. The silicone adhesive as described in claim 1, characterized in that, The crosslinking agent is prepared by reacting organosilicon monomer and pure water at a temperature of -10 to 40°C for 20 to 60 minutes in an inert atmosphere, and then reacting at a temperature of 100 to 150°C and a vacuum of (-0.097) to (-0.092) MPa for 30 to 90 minutes to obtain the crosslinking agent.

3. The silicone adhesive as described in claim 2, characterized in that, The organosilicon monomer is at least one of vinyltrimethoxysilane, vinyltriethoxysilane, methyltrimethoxysilane, methyltriethoxysilane, tetramethoxysilane, phenyltrimethoxysilane, γ-aminopropyltriethoxysilane, γ-aminopropyltrimethoxysilane, 3-aminopropylmethyldimethoxysilane, 3-aminopropylmethyldiethoxysilane, 3-(methacryloyloxy)propyltrimethoxysilane, and γ-[(2,3)-epoxypropyl]propyltrimethoxysilane; And / or, the mass of the purified water is 0.1-5 wt% of the mass of the organosilicon monomer.

4. The silicone adhesive as described in claim 1, characterized in that, The surface treatment agent also includes at least one of silane coupling agent and polyvinylpyrrolidone.

5. The silicone adhesive as described in claim 1, characterized in that, The polydimethylsiloxane is at least one of α,ω-dihydroxy polydimethylsiloxane, methyldimethoxy-terminated polydimethylsiloxane, trimethoxy-terminated polydimethylsiloxane, and vinyldimethoxy-terminated polydimethylsiloxane. And / or, the dynamic viscosity of the polydimethylsiloxane at 25°C is 750-20000 mPa·s.

6. The silicone adhesive as described in claim 1, characterized in that, The catalyst is at least one of dioctyltin diacetate, dioctyltin dilaurate, dioctyltin dioctate, dibutyltin diacetate, dibutyltin dilaurate, dibutyltin dioctate, isopropyl titanate, n-butyl titanate, ethyl acetoacetate chelate of isopropyl titanate, and acetylacetone chelate of isopropyl titanate. And / or, the first filler is at least one of thermally conductive filler and flame-retardant filler.

7. The method for preparing the silicone adhesive according to any one of claims 1-6, characterized in that, Includes the following steps: Polydimethylsiloxane and modified filler were dehydrated at 100-150℃ and under a vacuum of (-0.097)-(-0.092) MPa for 2-4 hours, then cooled to below 40℃, and crosslinking agent and catalyst were added. The mixture was stirred and reacted for 20-40 minutes to obtain silicone adhesive.

8. An elastomer, characterized in that, The elastomer is obtained by cross-linking and hardening the silicone adhesive according to any one of claims 1-6.

9. The use of the silicone adhesive as described in any one of claims 1-6 in the preparation of an insulating protective layer.