TW202124537A - Epoxy modified silicon resin composition and use thereof - Google Patents

Abstract

The present disclosure relates to an epoxy modified silicon resin composition and use thereof. The composition is prepared from raw materials of the following parts by weight: epoxy modified organic silicon resin 10 parts~70 parts, functional resin 10 parts~30 parts, auxiliary agent 15 parts~100 parts, and the epoxy modified organic silicon resin has a structure shown in Formula I, wherein R₁ is methyl, ethyl or phenyl; R₂ is methyl or phenyl; R₃ is methyl or phenyl; m is an integer in the range of 1~20; n is an integer in the range of 1~20.

Description

Epoxy modified silicone resin composition and its application

The present invention relates to the field of LED technology, in particular to epoxy-modified silicone resin compositions and their applications.

LED (Light-Emitting Diode), as a light source with small size, high luminous efficiency, low power consumption, and long service life, is widely used in fields such as display screens, lighting, and radiation sources. In recent years, with the development of LED miniaturization, thinning, and high-density trends, packaging methods that directly mount components on a printed wiring board have developed rapidly. With the development of high-brightness LED technology, LEDs have become more high-brightness, and at the same time, the heat generation of LED components has also increased. In the past, most of the substrates used to carry LED components were made of epoxy resin. However, epoxy resin has poor weather resistance and is exposed to high heat radiation for a long time, which causes the color of the substrate to age and turn yellow, and the reflectivity of light is reduced. , Which reduces the LED performance.

CN201410782137 discloses a yellowing resistant resin composition, the raw materials of which include: cycloaliphatic epoxy resin, general epoxy resin, cyanate ester resin, glycidyl methacrylate, curing agent, titanium dioxide, fluorescent whitening It has the advantages of good yellowing resistance, high reflectivity of the substrate, and high peel strength between the substrate and the metal foil. Adding cycloaliphatic epoxy resin directly, the weather resistance of the material is better than epoxy resin. However, the cost of alicyclic epoxy resin is high, and it is difficult to meet the increasingly stringent performance requirements.

CN201410829372 Compounds condensed silicone resins, catalysts, white fillers, additives, and optionally other components to obtain an organosilicon resin composition with excellent heat resistance, weather resistance and yellowing resistance. Silicone resin is used in the LED white copper-clad board to make it also have excellent heat resistance, weather resistance and yellowing resistance. However, the bonding strength of the material is poor.

Based on this, the present invention provides an epoxy-modified silicone resin composition, which has good mechanical properties, adhesive properties, excellent electrical insulation properties, and is resistant to high temperature aging, ultraviolet light, and radiation. The composition is a laminate prepared as a raw material, and when used as a substrate of an LED element, it can effectively improve the luminous effect of the LED and prolong the service life.

式I 其中，R₁ 為甲基、乙基或苯基； R₂ 為甲基或苯基； R₃ 為甲基或苯基； m為1-20範圍內的整數； n為1-20範圍內的整數。The specific technical method is: An epoxy-modified silicone resin composition prepared from raw materials including the following parts by weight: epoxy-modified organosilicon resin 10 parts to 70 parts, functional resin 10 parts to 30 parts, additives 15 parts to 100 parts, the epoxy-modified organosilicon resin has the structure shown in formula I:

Formula I Wherein, R ₁ is methyl, ethyl or phenyl; R ₂ is methyl or phenyl; R ₃ is methyl or phenyl; m is an integer in the range of 1-20; n is in the range of 1-20 Integer within.

The present invention also provides a prepreg. The raw material of the prepreg includes the above-mentioned epoxy-modified silicone resin composition.

The present invention also provides a laminate. The raw material of the laminate includes the above-mentioned epoxy-modified silicone resin composition or the above-mentioned prepreg.

Compared with the existing solutions, the present invention has the following beneficial effects: The epoxy-modified silicone resin composition of the present invention is prepared by using an epoxy-modified organosilicon resin having a specific structure of both epoxy groups and siloxy groups as one of the raw materials, together with functional resins and additives The epoxy-modified silicone resin composition can give full play to the good mechanical properties, bonding properties, and excellent electrical insulation properties of epoxy resins, and can also give full play to the high temperature aging resistance and ultraviolet light resistance of organosilicon resins. , Radiation resistance, laminates prepared with the epoxy modified silicone resin composition of the present invention as raw materials, compared with the traditional ordinary laminates, performance has been greatly improved, when used as the substrate of LED components, can be effective Improve the luminous effect of the LED and prolong the service life.

The present invention will be further described in detail below in conjunction with specific embodiments. The present invention can be implemented in many different forms and is not limited to the embodiments described herein. On the contrary, the purpose of providing these embodiments is to make the understanding of the disclosure of the present invention more thorough and comprehensive.

Unless otherwise defined, all technical and scientific terms used herein have the same meaning as commonly understood by those skilled in the technical field of the present invention. The terms used in the specification of the present invention herein are only for the purpose of describing specific embodiments, and are not intended to limit the present invention. The term "and/or" as used herein includes any and all combinations of one or more related listed items.

式I 其中， R₁ 為甲基、乙基或苯基； R₂ 為甲基或苯基； R₃ 為甲基或苯基； m為1-20範圍內的整數； n為1-20範圍內的整數。An epoxy-modified silicone resin composition is prepared from raw materials comprising the following parts by weight: epoxy-modified organosilicon resin 10 parts to 70 parts, functional resin 10 parts to 30 parts, auxiliary agent 15 parts to 100 parts , The epoxy-modified organosilicon resin has a structure shown in formula I:

Formula I Wherein, R ₁ is methyl, ethyl or phenyl; R ₂ is methyl or phenyl; R ₃ is methyl or phenyl; m is an integer in the range of 1-20; n is in the range of 1-20 Integer within.

The epoxy-modified silicone resin with the above-mentioned structure contains both epoxy groups and siloxy groups on the molecular chain, which not only has good mechanical properties, adhesion properties, excellent electrical insulation properties, and can withstand high temperature aging, Resistant to ultraviolet light and radiation.

Wherein, in the structure of the epoxy-modified silicone resin, the molar ratio of the organic substituent (R) to the silicon atom (Si), that is, the R/Si value, has a great effect on the quality of the epoxy-modified silicone resin. Relationship, will affect the curability of epoxy modified silicone resin, paint film flexibility, hardness, heat resistance and heat cracking resistance and other properties. Wherein, the organic substituent R represents the organic functional groups R ₁ , R ₂ , R ₃ , -C ₆ H ₅ and -CH _{3 in} the formula I, and the value of R/Si is R ₁ , R ₂ , R ₃ , -C The ratio of the total molar number of ₆ H ₅ and -CH _{3 to the molar number of silicon atoms.}

Preferably, the R/Si value is 1.5-2.0.

More preferably, the R/Si value is 1.75-1.85.

Preferably, the molecular weight of the epoxy-modified organosilicon resin is 1,000 to 30,000.

More preferably, the molecular weight of the epoxy-modified organosilicon resin is 1,000-15,000.

The preparation method of the above-mentioned epoxy-modified organosilicon resin is as follows: Mix 100-300 parts of tetramethyltetraphenylcyclotetrasiloxane monomer, 50-250 parts of T-link organosilicon monomer and 30-100 parts of end-capping agent, heat up to 50-80°C and reduce pressure to remove Water for 1 h-2 h, and then add 0.02%-0.08% of the total weight of the tetramethyltetraphenylcyclotetrasiloxane monomer, T-link organosilicon monomer and end-capping agent with an acid catalyst, and keep the temperature for reaction. 4 h-10 h, adjust the pH value to 6-7, filter and distill under reduced pressure to remove unreacted monomers to obtain vinyl-terminated organosilicon resin; Add 10-50 parts of oxidizing agent to 10-50 parts of the vinyl-terminated organosilicon resin at a temperature of -5-5℃, react at a temperature of 5-10℃ for 10 min-60 min, and then add 1-10 parts Reducing agent, stir for 10 min-60 min, and dry after extraction to obtain epoxy-modified silicone resin.

In the above preparation method, tetramethyltetraphenylcyclotetrasiloxane monomer, T-link organosilicon monomer (organosilicon trifunctional unit), and end-capping agent are used as reactive monomers. Under the action of an acid catalyst, First, a vinyl-terminated silicone resin was prepared. Then, the vinyl-terminated silicone resin prepared above is further oxidized with an oxidizing agent, and then a reducing agent is added to consume the excess oxidizing agent, and finally an epoxy-modified silicone resin is obtained, which avoids the epoxy resin, The compatibility problem between organosilicon resins, the preparation cost is low.

Understandably, the R/Si value can be adjusted by controlling the ratio of reaction monomers.

Preferably, 100-200 parts of tetramethyltetraphenylcyclotetrasiloxane monomer, 50-150 parts of T-link organosilicon monomer and 30-60 parts of end-capping agent are mixed, and the temperature is raised to 50-80°C After that, the water was removed under reduced pressure for 1 h-2 h, and then acidic acid which accounted for 0.02%-0.05% of the total weight of the tetramethyltetraphenylcyclotetrasiloxane monomer, T-link organosilicon monomer and capping agent was added. Catalyst, heat preservation reaction for 4 h-10 h, adjust the pH value to 6-7, filter and distill under reduced pressure to remove unreacted monomers to obtain vinyl-terminated organosilicon resin.

Preferably, the tetramethyltetraphenylcyclotetrasiloxane monomer is selected from 2,2,4,4-tetramethyl-6,6,8,8-tetraphenylcyclotetrasiloxane, 1,1,5,5-tetramethyl-1,3,3,5-tetraphenylcyclotetrasiloxane and 2,4,6,8-tetramethyl-2,4,6,8-tetra One or more of phenylcyclotetrasiloxane.

Preferably, the T-link organosilicon monomer is selected from methyl tris(dimethylsiloxyalkyl) silane, ethyl tris(dimethylsiloxyalkyl) silane, phenyl tris(dimethylsiloxane) Siloxyalkyl) Any of silanes.

Preferably, the capping agent is selected from 1,1,3,3-tetramethyl-1,3-divinyldisiloxane, 1,3-dimethyl-1,3-diphenyl Any one of -1,3-divinyldisiloxane and 1,1,3,3-tetraphenyl-1,3-divinyldisiloxane.

Preferably, the acid catalyst is selected from any one of sulfuric acid, phosphoric acid, trifluoromethanesulfonic acid and toluenesulfonic acid.

Preferably, the oxidant is selected from one or more of sodium hypochlorite and dilute sulfuric acid.

Preferably, the reducing agent is sodium sulfite.

封端劑終止聚合反應：

乙烯基環氧化：

。The synthetic route of the epoxy-modified organosilicon resin is as follows: Polymerization between monomers:

The capping agent terminates the polymerization reaction:

Vinyl epoxidation:

.

Understandably, the functional resin is selected from one or more of epoxy resin and bismaleimide.

The epoxy resin includes but is not limited to one of alicyclic epoxy resin, hydrogenated bisphenol A epoxy resin, glycidyl ester epoxy resin, cyanuric acid epoxy resin, hydantoin epoxy resin, etc. Many kinds.

The bismaleimide includes, but is not limited to, diphenylmethane bismaleimide, N'-m-phenylene dimaleimide (N, N'-m-phenylene dimaleimide), and polyamino bismaleimide One or more of maleimines.

The auxiliary agents are curing agents, fillers, coupling agents, curing accelerators, and the like.

In a preferred embodiment, the epoxy-modified silicone resin composition is prepared from raw materials including the following parts by weight: Epoxy modified silicone resin 10 parts-70 parts, Functional resin 10-30 copies, Curing agent 5-30 copies, Filler 10-60 copies, Coupling agent 0.1 part-2 part, Curing accelerator 0.1 part-2 part.

The curing agent includes, but is not limited to, cyanate ester curing agent, aliphatic polyamine curing agent, aromatic amine curing agent, polyamide curing agent, Lewis acid-amine complex curing agent, acid anhydride curing agent and One or more of phenolic curing agents, etc.

The filler includes, but is not limited to, one of titanium dioxide, silicon dioxide, magnesium oxide, magnesium hydroxide, talc, mica powder, aluminum oxide, silicon carbide, boron nitride, aluminum nitride, molybdenum oxide, and barium sulfate. Many kinds.

The coupling agent includes, but is not limited to, one or more of silane coupling agents, titanate coupling agents, aluminate coupling agents, and organic chromium complex coupling agents.

The curing accelerator includes, but is not limited to, imidazole accelerators, peroxide accelerators, azo accelerators, tertiary amine accelerators, phenol accelerators, organic metal salt accelerators, and inorganic metal salt accelerators One or more of etc.

A prepreg whose raw material includes the above-mentioned epoxy-modified silicone resin composition.

Understandably, the preparation method of the prepreg includes the following steps: The above-mentioned resin composition is covered on the surface of the reinforcing material by an impregnation method, and heated to semi-cured to obtain a prepreg.

Preferably, the program parameters of the semi-curing are: heating to a constant temperature of 130-250°C for 2 min-10 min.

It should be understood that the reinforcing material is a conventional inorganic or organic fiber material, and the inorganic fiber reinforced substrate includes but not limited to glass fiber (including E, NE, D, S, T and other types), carbon fiber, silicon carbide Fiber, asbestos fiber, etc. Organic fiber reinforced substrates include, but are not limited to, nylon, ultra-high molecular weight polyethylene fibers, aramid fibers, polyimide fibers, polyester fibers, cotton fibers, and the like.

A laminate, the raw material of which comprises the above-mentioned epoxy-modified silicone resin composition or the above-mentioned prepreg.

Understandably, the preparation method of the laminate includes the following steps: A number of the above-mentioned prepregs are laminated.

Preferably, the laminating program parameters are: under the conditions of temperature 150-300°C, pressure 10 kgf/cm ² -30 kgf/cm ² , and vacuum degree <2 kPa, hot pressing for 100 min-300 min.

The "a plurality of the prepregs" refers to at least one of the prepregs.

It should be noted that, during lamination, several prepregs, that is, one or both sides of the laminated body, can be coated with metal copper foil, and then laminated to obtain a metal copper foil-clad laminate.

Preferably, the thickness of the metal copper foil is 3 μm-35 μm.

The following will further illustrate in combination with specific examples. If there is no special description, all the raw materials in the present invention can be sourced from the market.

Hydrogenated bisphenol A epoxy resin can be purchased from Guodu Chemical, the model is ST-1000.

The cycloaliphatic epoxy resin can be purchased from Daicel, the model is 2021P.

The bismaleimide can be purchased from KI-Chemical, and the model is BMI-70.

Silicone resin can be purchased from Elecco, model SC2006.

Example 1 This embodiment provides a white epoxy-modified silicone resin composition, prepreg and laminate. The preparation method is as follows: Dissolve 70 parts of epoxy modified silicone resin, 10 parts of hydrogenated bisphenol A epoxy resin, and 5 parts of acid anhydride curing agent in a mixed solvent of methyl ethyl ketone, toluene and propylene glycol methyl ether. Among them, methyl ethyl ketone, toluene and Propylene glycol methyl ether is mixed in a mass ratio of 1:1:1. Under stirring conditions, add 10 parts of titanium dioxide, 25 parts of silicon dioxide, 0.1 parts of silane coupling agent and 2 parts of 2-methylimidazole, and continue to stir to obtain a uniform glue solution, namely epoxy modified silicone resin combination.

The 2116 glass fiber cloth (basis weight 105 g/m²) was impregnated in the epoxy-modified silicone resin composition and baked in a hot-air circulating oven at 180°C for 3 minutes to obtain a prepreg with a resin content of 50%.

Laminate 4 pieces of prepreg, and cover the upper and lower sides of the laminate with an electrolytic copper foil with a thickness of 12 μm, and place them in a vacuum press with programmable temperature and pressure. In a vacuum state, the temperature is 25 kgf/cm² Cured for 100 minutes at 200°C under the pressure of the same pressure to produce a copper-clad laminate with a thickness of 0.4 mm.

Example 2 This embodiment provides a white epoxy-modified silicone resin composition, prepreg and laminate. The preparation method is as follows: Dissolve 10 parts of epoxy-modified silicone resin, 30 parts of cycloaliphatic epoxy resin, and 30 parts of anhydride curing agent in a mixed solvent of methyl ethyl ketone, toluene and propylene glycol methyl ether. Among them, methyl ethyl ketone, toluene and propylene glycol Methyl ether is mixed in a mass ratio of 1:1:1. Under stirring conditions, add 10 parts of titanium dioxide, 10 parts of alumina, 40 parts of silicon dioxide, 2 parts of silane coupling agent and 0.1 parts of 2-methylimidazole, and continue to stir to obtain a uniform glue solution, namely Epoxy modified silicone resin composition.

The 2116 fiberglass cloth (basis weight 105 g/m²) was impregnated in the epoxy-modified silicone resin composition and baked in a hot-air circulating oven at 180°C for 3 minutes to obtain a prepreg with a resin content of 55%.

Laminate 4 pieces of prepreg, and cover the upper and lower sides of the laminate with an electrolytic copper foil with a thickness of 12 μm, and place them in a vacuum press with programmable temperature and pressure. In a vacuum state, the temperature is 25 kgf/cm² Cured for 100 minutes at 200°C under the pressure of the same pressure to produce a copper-clad laminate with a thickness of 0.4 mm.

Example 3 This embodiment provides a white epoxy modified silicone resin composition, prepreg and laminate, and the preparation method is as follows: Dissolve 50 parts of epoxy-modified silicone resin, 20 parts of bismaleimide, and 20 parts of phenolic curing agent in a mixed solvent of methyl ethyl ketone, toluene and propylene glycol methyl ether. Among them, methyl ethyl ketone, toluene and propylene glycol Methyl ether is mixed in a mass ratio of 1:1:1. Under stirring conditions, add 10 parts of titanium dioxide, 10 parts of alumina, 25 parts of silica, 0.5 parts of silane coupling agent, 0.5 parts of 2-methylimidazole and 0.7 parts of dicumyl peroxide, Continue to stir to obtain a uniform glue solution, that is, an epoxy-modified silicone resin composition.

The 2116 glass fiber cloth (basis weight 105 g/m²) was impregnated in the epoxy-modified silicone resin composition and baked in a hot-air circulating oven at 180°C for 3 minutes to obtain a prepreg with a resin content of 50%.

Laminate 4 pieces of prepreg, and cover the upper and lower sides of the laminate with an electrolytic copper foil with a thickness of 12 μm, and place them in a vacuum press with programmable temperature and pressure. In a vacuum state, the temperature is 25 kgf/cm² Cured for 100 minutes at 200°C under the pressure of the same pressure to produce a copper-clad laminate with a thickness of 0.4 mm.

Example 4 This embodiment provides a white epoxy-modified silicone resin composition, prepreg and laminate. The preparation method is as follows: Dissolve 50 parts of epoxy-modified silicone resin, 10 parts of cycloaliphatic epoxy resin, and 15 parts of anhydride curing agent in a mixed solvent of methyl ethyl ketone, toluene and propylene glycol methyl ether. Among them, methyl ethyl ketone, toluene and propylene glycol Methyl ether is mixed in a mass ratio of 1:1:1. Under stirring conditions, add 10 parts of titanium dioxide, 10 parts of alumina, 0.2 parts of silane coupling agent and 0.8 parts of 2-methylimidazole, and continue stirring to obtain a uniform glue solution, namely epoxy modified silicone resin combination Things.

The 2116 glass fiber cloth (basis weight 105 g/m²) was impregnated in the epoxy-modified silicone resin composition and baked in a hot-air circulating oven at 180°C for 3 minutes to obtain a prepreg with a resin content of 50%.

Laminate 4 pieces of prepreg, and cover the upper and lower sides of the laminate with an electrolytic copper foil with a thickness of 12 μm, and place them in a vacuum press with programmable temperature and pressure. In a vacuum state, the temperature is 25 kgf/cm² Cured for 100 minutes at 200°C under the pressure of the same pressure to produce a copper-clad laminate with a thickness of 0.4 mm.

Comparative example 1 This comparative example provides a white epoxy modified silicone resin composition, prepreg and laminate. The preparation method is as follows: Dissolve 40 parts of cycloaliphatic epoxy resin and 30 parts of acid anhydride curing agent in a mixed solvent of methyl ethyl ketone, toluene and propylene glycol methyl ether in sequence. Among them, methyl ethyl ketone, toluene and propylene glycol methyl ether are in a mass ratio of 1:1: 1 Mix. Under stirring conditions, add 10 parts of titanium dioxide, 10 parts of alumina, 40 parts of silicon dioxide, 2 parts of silane coupling agent and 0.1 parts of 2-methylimidazole, and continue to stir to obtain a uniform glue solution, namely Epoxy modified silicone resin composition.

The 2116 glass fiber cloth (basis weight 105 g/m²) was impregnated in the epoxy-modified silicone resin composition and baked in a hot-air circulating oven at 180°C for 3 minutes to obtain a prepreg with a resin content of 50%.

Laminate 4 pieces of prepreg, and cover the upper and lower sides of the laminate with an electrolytic copper foil with a thickness of 12 μm, and place them in a vacuum press with programmable temperature and pressure. In a vacuum state, the temperature is 25 kgf/cm² Cured for 100 minutes at 200°C under the pressure of the same pressure to produce a copper-clad laminate with a thickness of 0.4 mm.

Comparative example 2 This comparative example provides a white epoxy modified silicone resin composition, prepreg and laminate. The preparation method is as follows: Dissolve 100 parts of organosilicon resin and 1 part of dibutyltin dilaurate in a mixed solvent of methyl ethyl ketone, toluene and propylene glycol methyl ether. Among them, methyl ethyl ketone, toluene and propylene glycol methyl ether are in a mass ratio of 1:1:1 mix. Under stirring conditions, add 10 parts of titanium dioxide, 10 parts of alumina, and 0.7 parts of silane coupling agent, and continue to stir to obtain a uniform glue solution.

The 2116 fiberglass cloth (basis weight 105 g/m²) was dipped in the above glue and baked in a hot air circulating oven at 180°C for 3 minutes to obtain a prepreg with a resin content of 50%.

Laminate 4 pieces of prepreg, and cover the upper and lower sides of the laminate with an electrolytic copper foil with a thickness of 12 μm, and place them in a vacuum press with programmable temperature and pressure. In a vacuum state, the temperature is 25 kgf/cm² Cured for 100 minutes at 200°C under the pressure of the same pressure to produce a copper-clad laminate with a thickness of 0.4 mm.

Performance Testing Performance tests were performed on the products prepared in Examples 1-4 and Comparative Examples 1-2. The test methods are as follows, and the test results are shown in Table 1. Peel strength: The test method is carried out in accordance with IPC-TM-650 2.4.8. High temperature yellowing resistance test: the above copper-clad plate is etched to obtain a white laminate. The white laminate is cut into 4 inch*4 inch samples and placed in an oven at 200℃ for baking. The baking time is 4 h, 24 h, 72 h, and then test the reflectance and whiteness respectively, and compare with the unbaked sample. Weather resistance test: the above-mentioned copper-clad plate is etched to obtain a white laminate, and the white laminate is cut into 4 inch*4 inch samples, placed in a UV aging resistance test box, and placed at 85°C for 500 h , 750 h, 1000 h after testing the changes in reflectance and whiteness.

Table 1 Test items Example 1 Example 2 Example 3 Example 4 Comparative example 1 Comparative example 2 Peel strength/(lbf/in) 7.2 7.4 7.3 7.3 7.6 4.1 High temperature yellowing test BaiDu/% Before baking 92.0 92.0 91.6 91.8 91.3 90.7 4h 90.9 88.8 89.6 90.2 78.6 90.5 24h 88.7 86.6 87.7 88.3 75.1 90.2 72h 85.4 83.4 84.2 85.1 60.5 89.0 Reflectivity/% Before baking 94.6 94.3 94.1 94.3 95.3 94.5 4h 92.5 90.5 91.2 91.6 83.3 94.1 24h 90.2 88.1 89.2 89.4 81.4 93.0 72h 88.6 86.3 87.3 87.8 79.9 91.0 Weather resistance test BaiDu/% Before light 92.0 92.0 91.7 91.3 91.4 91.5 500h 88.2 86.5 87.4 87.5 81.2 90.0 750h 86.6 84.4 85.1 85.4 78.0 88.1 1000h 83.2 80.7 82.6 83.2 75.3 85.1 Reflectivity/% Before light 94.6 94.1 94.1 94.1 93.5 93.5 500h 92.5 90.2 91.0 91.6 85.0 93.0 750h 90.9 88.0 89.1 89.4 78.0 91.3 1000h 87.6 86.5 86.8 86.9 76.1 90.0 .

The epoxy-modified silicone resin composition prepared in Examples 1-4 has high peeling strength and good mechanical properties. After curing, it can maintain good whiteness for a long time. The laminate prepared by using it as a raw material has high High temperature yellowing resistance, weather resistance, used as the substrate of LED components, can effectively improve the luminous effect of the LED and prolong the service life.

Compared with Example 2, Comparative Example 1 did not add epoxy-modified silicone resin, but replaced it with an alicyclic epoxy resin of the same weight. While the cost increased, its high temperature yellowing resistance and weather resistance were far inferior. Example 2 illustrates that the addition of epoxy-modified silicone resin plays an important role in improving the weather resistance of the composition and even the laminate. Comparative Example 2 uses only organic silicon resin material, and its peel strength is poor.

The technical features of the above-mentioned embodiments can be combined arbitrarily. In order to make the description concise, all possible combinations of the various technical features in the above-mentioned embodiments are not described. However, as long as there is no contradiction in the combination of these technical features, All should be considered as the scope of this specification.

The above-mentioned embodiments only express several implementation modes of the present invention, and their description is relatively specific and detailed, but they should not be understood as a limitation on the patent scope of the present invention. It should be pointed out that for those of ordinary skill in the art, without departing from the concept of the present invention, several modifications and improvements can be made, and these all fall within the protection scope of the present invention. Therefore, the protection scope of the invention patent shall be subject to the scope of the attached invention application patent.

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Claims (12)

An epoxy-modified silicone resin composition, which is prepared from raw materials comprising the following parts by weight: epoxy-modified organosilicon resin 10 parts-70 parts, functional resin 10 parts-30 parts, auxiliary agent 15 parts- 100 parts, the epoxy-modified organosilicon resin has the structure shown in formula I:

Formula I Wherein, R ₁ is methyl, ethyl or phenyl; R ₂ is methyl or phenyl; R ₃ is methyl or phenyl; m is an integer in the range of 1-20; n is in the range of 1-20 Integer within. The epoxy-modified silicone resin composition according to claim 1, wherein the functional resin is selected from one or more of epoxy resin and bismaleimide. The epoxy-modified silicone resin composition according to claim 2, wherein the epoxy resin is selected from the group consisting of alicyclic epoxy resins, hydrogenated bisphenol A epoxy resins, glycidyl ester epoxy resins, and trimerized epoxy resins. One or more of cyanic acid epoxy resin and hydantoin epoxy resin. The epoxy-modified silicone resin composition according to claim 2, wherein the bismaleimide is selected from the group consisting of diphenylmethane bismaleimide and N'-m-phenylene bismaleimide (N,N'-m-phenylene dimaleimide) and one or more of polyamino bismaleimide. The epoxy-modified silicone resin composition according to any one of claims 1 to 4, wherein the auxiliary agent is selected from one or more of curing agents, fillers, coupling agents, and curing accelerators. The epoxy-modified silicone resin composition according to claim 5, which is prepared from raw materials including the following parts by weight: Epoxy modified silicone resin 10 parts-70 parts, Functional resin 10-30 copies, Curing agent 5-30 copies, Filler 10-60 copies, Coupling agent 0.1 part-2 part, Curing accelerator 0.1 part-2 part. The epoxy-modified silicone resin composition according to claim 6, wherein the curing agent is selected from the group consisting of cyanate ester curing agents, aliphatic polyamine curing agents, aromatic amine curing agents, polyamide curing agents, One or more of Lewis acid-amine complex curing agents, acid anhydride curing agents and phenolic curing agents. The epoxy-modified silicone resin composition according to claim 6, wherein the filler is selected from the group consisting of titanium dioxide, silicon dioxide, magnesium oxide, magnesium hydroxide, talc, mica powder, aluminum oxide, silicon carbide, nitriding One or more of boron, aluminum nitride, molybdenum oxide, and barium sulfate. The epoxy-modified silicone resin composition according to claim 6, wherein the coupling agent is selected from the group consisting of silane coupling agents, titanate coupling agents, aluminate coupling agents and organic chromium complex coupling agents One or more. The epoxy-modified silicone resin composition according to claim 6, wherein the curing accelerator is selected from the group consisting of imidazole accelerators, peroxide accelerators, azo accelerators, tertiary amine accelerators, One or more of phenolic accelerators, organic metal salt accelerators and inorganic metal salt accelerators. A prepreg, wherein the raw material of the prepreg comprises the epoxy-modified silicone resin composition according to any one of claims 1-10. A laminate, wherein the raw material of the laminate comprises the epoxy-modified silicone resin composition according to any one of claims 1-10, or the prepreg according to claim 11.