A non-yellowing silicone sealant and a method for preparing the same

Abstract

The application provides a silicone sealant not prone to discoloration and a preparation method thereof, and relates to the technical field of silicone sealants. The silicone sealant comprises the following components in parts by weight: 100 parts of hydroxyl-terminated polydimethylsiloxane, 70-130 parts of fillers, 0-20 parts of dimethyl silicone oil, 5-12 parts of a crosslinking agent, 1-3 parts of a coupling agent oligomer, 0.5-3 parts of an epoxy coupling agent and 0.01-0.5 parts of a catalyst. The application adopts a customized amino coupling agent oligomer with a specific structure, and optimizes the formula to achieve optimal effects by matching 107 glue, fillers and the like at a proper ratio. The application can improve the poor high-temperature tensile bonding property and the discoloration under high temperature of the existing silicone sealant, realizes good high-temperature bonding property and is not prone to discoloration, and in particular, the discoloration phenomenon under high-temperature application scenarios is obviously improved, thereby meeting the high requirements in special building, automobile, electronic and electrical applications and the like.

Description

TECHNICAL FIELD

[0001] The present application relates to the technical field of silicone sealant, in particular to a silicone sealant not prone to discoloration and a preparation method thereof. BACKGROUND

[0002] The silicone sealant is a sealant with excellent bonding performance, large mechanical strength, high elongation, resistance to ultraviolet light, ozone and weathering, electrical insulation and the like. At the same time, it has good bonding applicability and can be bonded with most materials, so it has great application value and wide application range, such as building, electronics and electrical fields. However, the silicone sealant is prone to discoloration after long-term use, especially under long-time sunshine and high temperature.

[0003] The discoloration of the silicone sealant is generally caused by the silane coupling agent KH550, KH792 and the like containing amino groups, which are prone to discoloration. The silane coupling agent containing amino groups is necessary in the silicone sealant, otherwise the bonding property will be obviously affected.

[0004] For example, patent application No. CN200910066244 discloses adding at least one of an ultraviolet light absorber, an antioxidant or a light stabilizer as an anti-yellowing agent to improve the anti-yellowing effect. CN201410510343 improves the weather resistance of the sealant by adding a composite anti-yellowing agent. CN201711086800 realizes the effects of anti-yellowing and mold resistance by adding a composite of bactericides and preservatives. CN201911276618 realizes the effects of anti-yellowing by designing a special structure of aging filler to absorb ultraviolet light and emit blue fluorescence, which offsets the visual yellowing effect.

[0005] However, the above existing patent technologies all add additives with ultraviolet light absorbers, antioxidants and the like or add light stabilizers and mold inhibitors to achieve the purpose of anti-yellowing. The above additives are generally organic macromolecules, which have poor compatibility with the silicone sealant system.

[0006] Patent application No. CN201410044556 discloses a method for testing yellowing at high temperature, which is aging at 100℃ for 48h. The temperature of the high-temperature treatment method in this technology is relatively low and the time is relatively short, and the long-term color stability at higher temperature is not concerned. In addition, the tensile bonding strength of the silicone sealant at high temperature is low, which cannot meet the specific requirements. At the same time, the silicone sealant is more prone to discoloration under high-temperature environment.

[0007] In summary, the existing technology lacks a solution for not discoloring and maintaining long-term tensile bonding under high-temperature application scenarios.

[0008] Based on the above problems, the patent proposes a silicone sealant with poor discoloration, especially at high temperature, and high temperature bonding resistance and a preparation method thereof. SUMMARY

[0009] The present application provides a silicone sealant with poor discoloration and a preparation method thereof, which aims to solve the poor high temperature tensile bonding and discoloration of existing silicone sealant.

[0010] In order to achieve the above purpose, the embodiment of the present application provides a silicone sealant with poor discoloration and a preparation method thereof, the present application adopts a customized specific structure of amino coupling agent oligomer, and optimizes the formula to match 107 glue, fillers and the like in a proper ratio, so as to achieve the optimal effect. The present application can improve the poor high temperature tensile bonding and discoloration of existing silicone sealant, realize poor discoloration and good high temperature bonding, especially the discoloration phenomenon in high temperature application scene is obviously improved, and meet the high requirements in special building, automobile, electronic and electrical appliances and other specific application occasions.

[0011] The embodiment of the present application provides a silicone sealant with poor discoloration, which comprises the following components in parts by weight:

[0012]

[0013] Preferably, the terminal hydroxyl group terminated polydimethylsiloxane has a viscosity of 3000-100000 mPa·s at 25℃.

[0014] Preferably, the filler is nano active calcium carbonate with a particle size of 80±20 nm and a cubic crystal form.

[0015] Preferably, the dimethyl silicone oil has a viscosity of 100-1000 mPa·s at 25℃.

[0016] Preferably, the crosslinking agent is selected from at least two of phenyl tributanone oxime silane, methyl tributanone oxime silane and tetrabutanone oxime silane.

[0017] Preferably, the coupling agent oligomer has the following general formula:

[0018]

[0019] In the formula, R1 is methyl, ethyl or propyl; R2 is an alkyl group with a carbon atom number of 5-20; R3 is methyl or ethyl; X is γ-aminopropyl, N-(β-aminoethyl)-γ-aminopropyl) or 3-(diethylenetriamine) propyl; and n is 3-9.

[0020] Preferably, X is gamma-aminopropyl in the coupling agent oligomer, R2 is alkyl with 5-20 carbon atoms, further, R2 is phenyl-containing alkyl with 7-20 carbon atoms; or, X is N-(beta-aminoethyl)-gamma-aminopropyl in the coupling agent oligomer, R2 is alkyl with 7-20 carbon atoms, further, R2 is alkyl with 9-20 carbon atoms, and more further, R2 is phenyl-containing alkyl with 9-20 carbon atoms; or, X is 3-(divinyltriamine) propyl in the coupling agent oligomer, R2 is alkyl with 11-20 carbon atoms, and further, R2 is phenyl-containing alkyl with 11-20 carbon atoms.

[0021] Preferably, the epoxy coupling agent is at least one of gamma-glycidoxypropyltrimeth(eth)oxy silane, epoxy cyclohexylmethyl dimeth(eth)oxy silane, 2-(3,4-epoxycyclohexyl) ethyl trimeth(eth)oxy silane, and gamma-(2,3-epoxypropoxy) propyl trimethoxy siloxane.

[0022] Preferably, the catalyst is at least one of dibutyltin dilaurate, dibutyltin diacetate, and dibutyltin dioctate.

[0023] Based on the general concept of an invention, embodiments of the present application provide the preparation method of the above-mentioned silicone sealant not prone to discoloration, comprising the following steps:

[0024] S1: according to the proportion, stirring the hydroxyl-terminated polydimethylsiloxane, filler, and dimethyl silicone oil uniformly, vacuum dewatering for 2-4 hours, dewatering temperature 90-140 DEG C, vacuum degree -0.09-0.1 MPa, and cooling to room temperature to obtain a base material;

[0025] S2: according to the proportion, adding the base material, crosslinking agent, coupling agent oligomer, epoxy coupling agent, and catalyst in a high-speed planetary mixer, and vacuum stirring under a vacuum degree of -0.075-0.095 MPa to obtain the silicone sealant not prone to discoloration.

[0026] The above-mentioned scheme of the present application has the following beneficial effects:

[0027] (1) The present application adopts a unique amino coupling agent oligomer, and the long-chain alkane structure beside the amino silane with an alternating copolymer structure can greatly reduce the discoloration of the amino group. Further, the branched structure of the long-chain alkane containing phenyl can significantly improve the high-temperature resistance, and is less prone to discoloration, especially at high temperatures, which is more excellent than the silicone sealant using KH550, KH792, etc. as the coupling agent.

[0028] (2) The amino coupling agent oligomer of the present application is still a silicone structure, and is compatible with a silicone adhesive system, and the anti-discoloration effect of the sealant is more persistent and stable. At the same time, because the oligomer structure contains more reactive groups, the adhesion is also significantly improved, especially the tensile adhesion in a high-temperature environment is better maintained. Furthermore, the tensile adhesion of the di- and tri-amino silane oligomer is better, because the coupling agent molecular chain is longer, the amino groups are more, and the molecular structure formula contains both primary and secondary amine groups. DETAILED DESCRIPTION

[0029] In order to make the technical problems, technical solutions and advantages of the present application clearer, specific embodiments will be described in detail below.

[0030] Unless otherwise defined, all the professional terms used below have the same meaning as generally understood by those skilled in the art. The professional terms used in the present application are only for the purpose of describing specific embodiments, and are not intended to limit the protection scope of the present application.

[0031] Unless otherwise specified, various raw materials, reagents, instruments and equipment used in the present application can be purchased from the market or can be prepared by existing methods.

[0032] The present application provides a silicone sealant which is not easy to discolor, and includes the following components by weight:

[0033]

[0034] Preferably, the terminal hydroxyl group terminated polydimethylsiloxane has a viscosity of 3000-100000 mPa·s at 25℃.

[0035] Preferably, the filler is nano active calcium carbonate with a particle size of 80±20 nm and a cubic crystal form.

[0036] Preferably, the dimethyl silicone oil has a viscosity of 100-1000 mPa·s at 25℃.

[0037] Preferably, the crosslinking agent is selected from at least two of phenyl tributanone oxime silane, methyl tributanone oxime silane and tetrabutanone oxime silane.

[0038] Preferably, the coupling agent oligomer has the following general formula:

[0039]

[0040] In the formula, R1 is methyl, ethyl or propyl; R2 is an alkyl group with a carbon atom number of 5-20; R3 is methyl or ethyl; X is γ-aminopropyl, N-(β-aminoethyl)-γ-aminopropyl) or 3-(diethylenetriamine group) propyl; and n is 3-9.

[0041] Preferably, X is γ-aminopropyl, R2 is alkyl with 5-20 carbon atoms, further, R2 is phenyl-containing alkyl with 7-20 carbon atoms; or, X is N-(β-aminoethyl)-γ-aminopropyl, R2 is alkyl with 7-20 carbon atoms, further, R2 is alkyl with 9-20 carbon atoms, and more further, R2 is phenyl-containing alkyl with 9-20 carbon atoms; or, X is 3-(divinyltriamine) propyl, R2 is alkyl with 11-20 carbon atoms, further, R2 is phenyl-containing alkyl with 11-20 carbon atoms.

[0042] Preferably, the epoxy coupling agent is at least one of γ-glycidoxypropyltrimeth(eth)oxy silane, epoxy cyclohexylmethyl dimeth(eth)oxy silane, 2-(3,4-epoxycyclohexyl) ethyl trimeth(eth)oxy silane, and γ-(2,3-epoxypropoxy) propyl trimethoxy siloxane.

[0043] Preferably, the catalyst is at least one of dibutyltin dilaurate, dibutyltin diacetate, and dibutyltin dioctate.

[0044] Based on the general concept of an invention, embodiments of the present application provide the above-mentioned preparation method of the silicone sealant not prone to discoloration, comprising the following steps:

[0045] S1: according to the ratio, stirring the hydroxyl-terminated polydimethylsiloxane, fillers, and dimethyl silicone oil uniformly, vacuum dewatering for 2-4 hours, dewatering temperature 90-140℃, vacuum degree -0.09-0.1 MPa, and cooling to room temperature to obtain a base material;

[0046] S2: according to the ratio, adding the base material, crosslinking agent, coupling agent oligomer, epoxy coupling agent, and catalyst in a high-speed planetary mixer, and vacuum stirring under a vacuum degree of -0.075-0.095 MPa to obtain the silicone sealant not prone to discoloration.

[0047] The coupling agent oligomer in the following examples is customized by Shandong Silicon New Material Co., Ltd. The following is illustrated by specific examples.

[0048] Example 1

[0049] The present embodiment provides a preparation method of a silicone sealant not prone to discoloration, comprising the following steps:

[0050] (1) stirring 100 parts of 50000 mPa·s hydroxyl-terminated polydimethylsiloxane and 70 parts of nano calcium carbonate uniformly, vacuum dewatering for 3 hours, dewatering temperature 100℃, vacuum degree -0.095 MPa, and cooling to room temperature to obtain a base material;

[0051] (2) In the high-speed planetary mixer, the above-mentioned base material, methyltris(butanone oxime) silane 6 parts, phenyltris(butanone oxime) silane 3 parts, custom-made coupling agent oligomer (R1 is methyl; R2 is heptyl; R3 is ethyl; X is N-(β-aminoethyl)-γ-aminopropyl); n = 3) 2.5 parts, γ-glycidyl ether oxypropyl triethoxysilane 1 part, dibutyltin dilaurate 0.1 part are added, vacuum stirring is carried out under the vacuum degree of -0.085 MPa, and then the silicone sealant is obtained.

[0052] Example 2

[0053] The embodiment provides a preparation method of a silicone sealant which is not easy to discolor, and the method comprises the following steps:

[0054] (1) 10000 mPa·s hydroxyl-terminated polydimethylsiloxane 100 parts, nano calcium carbonate 90 parts, and dimethyl silicone oil 5 parts are uniformly stirred, vacuum dehydration is carried out for 2 hours, the dehydration temperature is 120 DEG C, the vacuum degree is -0.090 MPa, and after cooling to room temperature, a base material is obtained;

[0055] (2) In the high-speed planetary mixer, the above-mentioned base material, methyltris(butanone oxime) silane 7 parts, phenyltris(butanone oxime) silane 1.5 parts, custom-made coupling agent oligomer (R1 is propyl; R2 is dodecyl; R3 is methyl; X is 3-(diethylenetriamine) propyl; n = 5) 3 parts, cyclohexyl epoxy methyl dimethoxysilane 1.2 parts, and dibutyltin dilaurate 0.5 parts are added, vacuum stirring is carried out under the vacuum degree of -0.095 MPa, and then the silicone sealant is obtained.

[0056] Example 3

[0057] The embodiment provides a preparation method of a silicone sealant which is not easy to discolor, and the method comprises the following steps:

[0058] (1) 80000 mPa·s hydroxyl-terminated polydimethylsiloxane 100 parts, nano calcium carbonate 100 parts, and dimethyl silicone oil 8 parts are uniformly stirred, vacuum dehydration is carried out for 4 hours, the dehydration temperature is 140 DEG C, the vacuum degree is -0.1 MPa, and after cooling to room temperature, a base material is obtained;

[0059] (2) In the high-speed planetary mixer, the above-mentioned base material, methyltris(butanone oxime) silane 8 parts, tetrabutanone oxime silane 2 parts, custom-made coupling agent oligomer (R1 is methyl; R2 is a linear long-chain alkyl group with 19 carbon atoms; R3 is methyl; X is γ-aminopropyl; n = 7) 2.8 parts, 2-(3,4-epoxycyclohexyl) ethyl trimethoxysilane 1 part, and dibutyltin dilaurate 0.3 parts are added, vacuum stirring is carried out under the vacuum degree of -0.088 MPa, and then the silicone sealant is obtained.

[0060] Example 4

[0061] The embodiment provides a preparation method of a silicone sealant which is not prone to discoloration, and comprises the following steps:

[0062] (1) uniformly stir 100 parts of 50000 mPa·s end-hydroxyl terminated polydimethylsiloxane, 110 parts of nano calcium carbonate and 10 parts of dimethyl silicone oil, vacuumize and dehydrate for 3 hours, the dehydration temperature is 130 DEG C, the vacuum degree is -0.096 MPa, and after cooling to room temperature, a base material is obtained;

[0063] (2) in a high-speed planetary stirrer, the base material, 4 parts of methyl tributanone oxime silane, 4 parts of phenyl tributanone oxime silane, 2.5 parts of a customized coupling agent oligomer (R1 is ethyl; R2 is phenyl nonyl; R3 is methyl; X is 3-(diethylene triamine) propyl; n=6), 0.8 parts of gamma-glycidyl ether oxygen propyl trimethoxysilane and 0.2 parts of dibutyl tin dilaurate are added, vacuum stirring is conducted under a vacuum degree of -0.093 MPa, and the silicone sealant which is not prone to discoloration is obtained.

[0064] Example 5

[0065] The embodiment provides a preparation method of a silicone sealant which is not prone to discoloration, and comprises the following steps:

[0066] (1) uniformly stir 100 parts of 100000 mPa·s end-hydroxyl terminated polydimethylsiloxane, 120 parts of nano calcium carbonate and 16 parts of dimethyl silicone oil, vacuumize and dehydrate for 3 hours, the dehydration temperature is 135 DEG C, the vacuum degree is -0.098 MPa, and after cooling to room temperature, a base material is obtained;

[0067] (2) in a high-speed planetary stirrer, the base material, 9 parts of methyl tributanone oxime silane, 3 parts of tetrabutanone oxime silane, 0.5 parts of a customized coupling agent oligomer (R1 is methyl; R2 is phenyl pentyl; R3 is ethyl; X is gamma-aminopropyl; n=9), 2 parts of gamma-glycidyl ether oxygen propyl trimethoxysilane and 0.01 parts of dibutyl tin diacetate are added, vacuum stirring is conducted under a vacuum degree of -0.090 MPa, and the silicone sealant which is not prone to discoloration is obtained.

[0068] Example 6

[0069] The embodiment provides a preparation method of a silicone sealant which is not prone to discoloration, and comprises the following steps:

[0070] (1) uniformly stir 100 parts of 20000 mPa·s end-hydroxyl terminated polydimethylsiloxane, 130 parts of nano calcium carbonate and 20 parts of dimethyl silicone oil, vacuumize and dehydrate for 3.5 hours, the dehydration temperature is 125 DEG C, the vacuum degree is -0.093 MPa, and after cooling to room temperature, a base material is obtained;

[0071] (2) In a high speed planetary mixer, the above base material, methyltris(tributylketoximo)silane 8.5 parts, tetrabutylketoximosilane 1.5 parts, custom coupling agent oligomer (R1 is methyl; R2 is phenyltetradecyl; R3 is methyl; X is N-(β-aminoethyl)-γ-aminopropyl); n = 8) 1 part, 2-(3,4-epoxycyclohexyl)ethyltrimethoxysilane 3 parts, dibutyltin diacetate 0.05 parts were added, and vacuum stirring was carried out under a vacuum degree of -0.091 MPa to obtain the silicone sealant.

[0072] Example 7

[0073] This example is basically the same as Example 1, except that the custom coupling agent oligomer (R1 is methyl; R2 is nonyl; R3 is ethyl; X is N-(β-aminoethyl)-γ-aminopropyl); n = 3) 2.5 parts.

[0074] Example 8

[0075] This example is basically the same as Example 1, except that the custom coupling agent oligomer (R1 is methyl; R2 is phenylpropyl; R3 is ethyl; X is N-(β-aminoethyl)-γ-aminopropyl); n = 3) 2.5 parts.

[0076] Comparative Example 1

[0077] This comparative example is basically the same as Example 3, except that KH550 is used instead of the coupling agent oligomer.

[0078] Comparative Example 2

[0079] This comparative example is basically the same as Example 4, except that 3-(divinyltriamino)propyltrimethoxysilane is used instead of the coupling agent oligomer.

[0080] The sample preparation and performance testing were carried out according to GB 16776 to test after sample preparation and curing. The performance test data of the silicone sealants of Examples 1-8 and Comparative Examples 1-2 above are shown in Tables 1, 2, and 3.

[0081] Measurement of color change after artificial acceleration:

[0082] (1) The sample was prepared and the color change degree was measured according to GB / T 13477.21, and the color change degree was divided into 0-3 levels according to the color change level in the standard, wherein 0 level means no color change, and 3 level means obvious color change as the highest level.

[0083] (2) High temperature acceleration method: the sample prepared and cured according to GB / T 13477.21 was placed in an oven at 200°C for a period of time (7, 28, 56 days), and the color change degree was observed according to the above method,

[0084] Tensile adhesion after high temperature aging:

[0085] High temperature aging treatment method: the finished I-beam is placed in a 200°C oven for a period of time (7, 28, 56 days), and then placed at room temperature for 24h. Its tensile adhesion is detected according to GB 16776.

[0086] Table 1

[0087]

[0088] Table 2

[0089]

[0090] Table 3

[0091]

[0092] From the above examples and comparative examples, it can be seen that the discoloration grades of examples 1-8 are significantly lower than those of comparative examples 1-2, indicating that the use of the coupling agent oligomer described in the patent can significantly improve the discoloration of the silicone sealant.

[0093] By comparing the effects of example 3 and comparative example 1, it can be seen that under the irradiation conditions specified in GB / T 13477.21, the silicone sealant of comparative example 1 gradually becomes more and more discolored with the extension of irradiation time, while the silicone sealant of example 3 remains unchanged. At the same time, under high temperature conditions, the silicone sealant of comparative example 1 is more prone to discoloration, while the silicone sealant of example 3 can still remain unchanged.

[0094] By comparing the effects of example 4 and comparative example 2, it can be seen that under the irradiation conditions specified in GB / T 13477.21, the silicone sealant of comparative example 2 gradually becomes more and more discolored with the extension of irradiation time, and it discolored faster than comparative example 1, while the silicone sealant of example 4 remains unchanged, still maintaining the anti-discoloration ability of example 3. At the same time, under high temperature conditions, the silicone sealant of comparative example 2 discolors obviously at the beginning, while the silicone sealant of example 4 can still remain unchanged, still maintaining the anti-discoloration ability of example 3. At the same time, its high temperature tensile adhesion strength is relatively improved more obviously than example 3, indicating that the side chain structure of phenyl alkyl has obvious effect on anti-discoloration and tensile adhesion improvement under high temperature application scenarios.

[0095] By comparing examples 1-3, although the discoloration degree is smaller than that of comparative example 1, there is still some difference, which shows that the length of the long-chain alkane side chain also has some effect: examples 2-3 with longer carbon chain structure are better than example 1.

[0096] By comparing the comparative examples 1, 7, 8, it is more clearly shown that the long chain side chain of the preferred longer alkyl structure performs better in the aspect of not easy to discolor, the long chain side chain containing phenyl structure performs more excellent in the aspect of not easy to discolor, and the high-temperature tensile bonding strength is also better.

[0097] By comparing the comparative examples 1-3 and 4-6, it is shown that the long chain side chain containing phenyl structure performs more excellent in the aspect of not easy to discolor, and the high-temperature tensile bonding strength is also better.

[0098] The above is the preferred embodiment of the present application, it should be pointed out that, for the ordinary skilled in the art, without departing from the principles of the present application, can also make a number of improvements and refinements, these improvements and refinements should also be considered as the protection scope of the present application.

Claims

1. A non-yellowing silicone sealant, characterized by, comprising the following components by weight parts: The coupling agent oligomer has the following general formula: wherein R1 is methyl, ethyl or propyl; R2 is alkyl with 5-20 carbon atoms; R3 is methyl or ethyl; X is γ-aminopropyl, N-(β-aminoethyl)-γ-aminopropyl) or 3-(diethylenetriamine) propyl; and n is 3-9.

2. The non-yellowing silicone sealant according to claim 1, wherein The terminal hydroxyl group terminated polydimethylsiloxane has a viscosity of 3000-100000 mPa·s at 25℃.

3. The non-yellowing silicone sealant of claim 1, wherein The filler is nano active calcium carbonate with a particle size of 80±20 nm and cubic crystal form.

4. The non-yellowing silicone sealant of claim 1, wherein The dimethyl silicone oil has a viscosity of 100-1000 mPa·s at 25℃.

5. The non-yellowing silicone sealant of claim 1, wherein The crosslinking agent is selected from at least two of phenyltributanoxysilane, methyltributanoxysilane and tetrabutanoxysilane.

6. The non-yellowing silicone sealant of claim 1, wherein In the coupling agent oligomer, X is γ-aminopropyl and R2 is alkyl with 5-20 carbon atoms; Alternatively, in the coupling agent oligomer, X is N-(β-aminoethyl)-γ-aminopropyl) and R2 is alkyl with 7-20 carbon atoms; Alternatively, in the coupling agent oligomer, X is 3-(diethylenetriamine) propyl and R2 is alkyl with 11-20 carbon atoms.

7. The non-yellowing silicone sealant of claim 1, wherein The epoxy coupling agent is at least one of γ-glycidyloxypropyltrimeth(eth)oxysilane, epoxy cyclohexylmethyl dimeth(eth)oxysilane, 2-(3,4-epoxycyclohexyl) ethyl trimeth(eth)oxysilane and γ-(2,3-epoxypropoxy) propyl trimethoxysiloxane.

8. The non-yellowing silicone sealant of claim 1, wherein The catalyst is at least one of dibutyltin dilaurate, dibutyltin diacetate and dibutyltin dioctate.

9. The process for producing a non-yellowing silicone sealant according to any one of claims 1 to 8, characterized in that, The method comprises the following steps: S1: uniformly stirring the terminal hydroxyl group terminated polydimethylsiloxane, filler and dimethyl silicone oil according to the proportions, vacuum dewatering for 2-4 h at a dewatering temperature of 90-140℃ and a vacuum degree of -0.09-0.1 MPa, and cooling to room temperature to obtain a base material; S2: adding the base material, crosslinking agent, coupling agent oligomer, epoxy coupling agent and catalyst into a high-speed planetary mixer according to the proportions, and vacuum stirring at a vacuum degree of -0.075-0.095 MPa to obtain the product.

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