Preparation method and application of heteropolyacid siloxane glycidyl ether composite material

Abstract

The invention discloses a preparation method and application of a heteropolyacid siloxane glycidyl ether composite material, and belongs to the technical field of preparation of organic and inorganic composites.The preparation method comprises the steps that heteropolyacid is dispersed in solvent xylene or methylbenzene, an amino silane coupling agent is dropwise added, reduced pressure distillation and drying are conducted after reaction, and a solid product is obtained; the preparation method comprises the following steps: dispersing an alkyl glycidyl ether solution, a silane coupling agent, a silane coupling agent, a silane coupling agent, a silane coupling agent, a silane coupling agent, a silane coupling agent, a silane coupling agent, a silane coupling agent, a silane coupling agent, a silane coupling agent, a silane coupling agent, a silane coupling agent, a silane coupling agent, a silane coupling agent, a silane coupling agent, a silane coupling agent, a silane coupling agent and a silane coupling agent into an alkyl glycidyl ether solution, and carrying out reduced pressure distillation and drying to obtain the product. According to the present invention, the surface organosilicon coating is formed, the performance of the heteropolyacid as the heat-resistant additive is improved, the heteropolyacid siloxane interacts with the phenyl glycidyl ether or the octyl glycidyl ether, the phenyl glycidyl ether or the octyl glycidyl ether further modifies the heteropolyacid siloxane, and the heat resistance is substantially improved.

Description

Technical field:

[0001] The invention belongs to the technical field of preparation of organic and inorganic composite materials, and particularly relates to a preparation method of a heteropolyacid siloxane glycidyl ether composite material and application of a heat-resistant agent. Background technology:

[0002] Epoxy resin adhesives are widely used in coatings, construction, aerospace, high-speed rail and other fields. They have the advantages of fast bonding speed, high bonding strength, acid and alkali resistance, and high hardness. Epoxy resin adhesives are usually two-component, with component A mainly composed of epoxy resin, fillers, and additives, and component B mainly composed of amino curing agents. With the improvement of scientific and technological levels, higher performance requirements are put forward for epoxy resin adhesives used in extreme environments. In particular, with the rapid development of new energy, epoxy resin adhesives that can be used under high temperature conditions have attracted much attention.

[0003] One of the main means to improve the heat resistance of epoxy resin is to compound it with silicone materials. The invention patent (CN201910884583.1) improves the heat resistance of epoxy resin by constructing a block interconversion network of the epoxy resin base polymer, and adopts block modification between silicone rubber. In addition, the simplest way to improve the heat resistance of epoxy resin is to add heat-resistant additives directly to the epoxy resin. For example, using polysilsesquioxane (POSS) as an additive can improve the heat resistance of epoxy resin (invention patent CN202410150760.4); using phosphazene compounds as additives for epoxy resin improves the flame retardancy and heat resistance of epoxy resin (invention patent CN200680007911.0). However, the incompatibility between the additive and the epoxy resin can cause the additive to precipitate or cause the powder to agglomerate, resulting in uneven dispersion and affecting the heat resistance. The invention patent (CN202311173521.2) uses a C=C-containing epoxy monomer and a hydrogen-containing silicone resin through a platinum-catalyzed addition reaction to wrap the surface of the silicone resin with a carbon-based polymer to prepare an epoxy group-modified silicone resin, which is used as a heat-resistant additive for epoxy resin.

[0004] Heteropolyacid structures also have potential uses as heat-resistant additives for epoxy resins. For example, the invention patent (CN202210546849.3) discloses a zinc-containing Anderson-type heteropolyacid flame retardant and smoke suppressant, which drives the self-aggregation of POMs hybrid molecules in the epoxy matrix to form a nanoscale microscopic phase or topological structure, thereby achieving the purpose of nano-enhancement, and is expected to achieve comprehensive performance improvements in epoxy resins such as flame retardancy, mechanics, heat resistance, and dielectric properties.

[0005] However, there are still huge challenges in designing new structures, enhancing the compatibility of additives with epoxy resins, and obtaining epoxy resins with high heat resistance. Summary of the invention:

[0006] In order to solve the above problems and overcome the shortcomings of the prior art, the present invention provides a heteropolyacid siloxane glycidyl ether composite material that can be used as a heat-resistant agent, which can effectively solve the problems of poor compatibility with epoxy resin and poor heat resistance.

[0007] The specific technical solution of the present invention to solve the above technical problem is: a method for preparing a heteropolyacid siloxane glycidyl ether composite material, characterized in that the preparation of the heteropolyacid siloxane glycidyl ether composite material comprises the following steps:

[0008] (1) dispersing a heteropoly acid in a solvent of xylene or toluene, adding an aminosilane coupling agent dropwise, distilling under reduced pressure after the reaction, and drying to obtain a solid product; the heteropoly acid is a phosphotungstic acid aqueous solution or a phosphomolybdic acid ethanol solution;

[0009] (2) The solid powder is dispersed in a solution of alkyl glycidyl ether, reacted at a certain temperature, and then distilled under reduced pressure and dried to obtain a product.

[0010] Furthermore, in step (1), the mass fraction of the phosphotungstic acid aqueous solution is 5-20wt%; the mass fraction of the phosphomolybdic acid ethanol solution is 5-20wt%.

[0011] Furthermore, in step (1), the aminosilane coupling agent is any one of aminopropyltrimethoxysilane, aminopropyltriethoxysilane, aminopropylmethyldimethoxysilane and aminopropylmethyldiethoxysilane.

[0012] Furthermore, in step (1), the reaction temperature is 40-60°C and the reaction time is 12-24h.

[0013] Furthermore, the molar ratio of the heteropoly acid to the aminosilane coupling agent is 1:(3-5).

[0014] Furthermore, in step (2), the alkane glycidyl ether is phenyl glycidyl ether or octyl glycidyl ether.

[0015] Furthermore, in step (2), the mass fraction of the alkyl glycidyl ether solution is 5-10wt%, and the molar number of the alkyl glycidyl ether is 1-1.5 times that of the aminosilane coupling agent.

[0016] Furthermore, in step (2), the reaction temperature is 70-100° C. and the reaction time is 2-5 h.

[0017] The heteropolyacid siloxane glycidyl ether composite material is prepared by adopting the preparation method of the heteropolyacid siloxane glycidyl ether composite material, and is characterized in that the heteropolyacid siloxane glycidyl ether composite material is used as an epoxy resin heat resistant agent.

[0018] The beneficial effects of the present invention are:

[0019] The present invention utilizes the hydrolysis and polycondensation reaction of an aminosilane coupling agent to graft silane alkoxy groups into the structure of a heteropoly acid, thereby forming a chemical combination between the surface of the heteropoly acid and the silanol group, forming a surface organic silicon coating, and improving the performance of the heteropoly acid as a heat-resistant additive. The heteropoly acid siloxane interacts with phenyl glycidyl ether or octyl glycidyl ether, and the phenyl glycidyl ether or octyl glycidyl ether further modifies the heteropoly acid siloxane, thereby greatly improving the heat resistance. Description of the drawings:

[0020] Attached Figure 1 is the infrared spectrum of the composite material prepared by the present invention;

[0021] Attached Figure 2 This is a state diagram of the composite material prepared by the present invention after adding epoxy resin;

[0022] Attached Figure 3 This is a state diagram of the composite material prepared in Comparative Example 1 after epoxy resin is added;

[0023] Attached Figure 4 This is a thermogravimetric spectrum of pure epoxy resin, a composite material prepared by the present invention; Specific implementation method:

[0024] In the description of the present invention, specific details are only for a full understanding of the embodiments of the present invention, but those skilled in the art should know that the implementation of the present invention is not limited to these details. In addition, well-known structures and functions are not described or shown in detail to avoid blurring the key points of the embodiments of the present invention. For those of ordinary skill in the art, the specific meanings of the above terms in the present invention can be understood according to specific circumstances.

[0025] Specific implementation of the present invention:

[0026] In order to better understand the present invention, a specific embodiment is used for illustration. It is worth emphasizing that the effect of this embodiment is not substantially different from the various embodiments within the protection scope of the present invention, including the respective reagents and the content ratio of the reagents, and all of them can achieve the effects described in the present invention and solve the above-mentioned problems. Other combinations are not described here.

[0027] Embodiment 1:

[0028] (1) Take 216 g of phosphotungstic acid aqueous solution (mass fraction 15 wt%), add 10 g of aminopropyltriethoxysilane dropwise under magnetic stirring, react at 50° C. for 18 h, and then evaporate the water under reduced pressure to obtain a white powder.

[0029] (2) The white powder was added to a solution of 11 g of octyl glycidyl ether and 135 g of xylene, and the temperature was raised to 85° C. with magnetic stirring and kept for 3 h, then cooled to room temperature and dried under reduced pressure to obtain the product.

[0030] (3) Add 5% of the above solid powder into epoxy resin for curing.

[0031] Embodiment 2:

[0032] (1) 136 g of ethanol solution of phosphomolybdic acid (mass fraction 15 wt%) was added dropwise with 10 g of aminopropyltriethoxysilane under magnetic stirring, and the mixture was reacted under reflux at 60° C. for 24 h, and then the mixture was decompressed and degassed.

[0033] (2) The above product was added to a solution of 11 g of octyl glycidyl ether and 135 g of xylene, and the temperature was raised to 85° C. with magnetic stirring and kept for 3 h, then cooled to room temperature and dried under reduced pressure to obtain the product.

[0034] (3) Add 5% of the above solid powder into epoxy resin for curing.

[0035] Embodiment 3:

[0036] (1) Take 216 g of phosphotungstic acid aqueous solution (mass fraction 15 wt%), add 10 g of aminopropyltriethoxysilane dropwise under magnetic stirring, react at 50° C. for 18 h, and then evaporate the water under reduced pressure to obtain a white powder.

[0037] (2) The white powder was added to a solution of 9 g of phenyl glycidyl ether and 120 g of toluene, and the temperature was raised to 80° C. with magnetic stirring and kept for 3 h, then cooled to room temperature and dried under reduced pressure to obtain the product.

[0038] (3) Add 5% of the above solid powder into epoxy resin for curing.

[0039] Embodiment 4:

[0040] (1) 136 g of ethanol solution of phosphomolybdic acid (mass fraction 15 wt%) was added dropwise with 10 g of aminopropylmethyldiethoxysilane under magnetic stirring, and the mixture was reacted under reflux at 60° C. for 24 h, and then decompressed to remove the precipitate.

[0041] (2) The above product was added to a solution of 9 g of octyl glycidyl ether and 120 g of xylene, and the temperature was raised to 80° C. with magnetic stirring and kept for 3 h, then cooled to room temperature and dried under reduced pressure to obtain the product.

[0042] (3) Add 5% of the above solid powder into epoxy resin for curing.

[0043] Embodiment 5:

[0044] (1) Take 216 g of phosphotungstic acid aqueous solution (mass fraction 15 wt%), add 12.4 g of aminopropyltrimethoxysilane dropwise under magnetic stirring, react at 60° C. for 12 h, and then evaporate the water under reduced pressure to obtain a white powder.

[0045] (2) The white powder was added to a solution of 15.7 g of octyl glycidyl ether and 140 g of xylene, and the temperature was raised to 100° C. under magnetic stirring and reflux for 2 h, then cooled to room temperature and dried under reduced pressure to obtain the product.

[0046] (3) Add 5% of the above solid powder into epoxy resin for curing.

[0047] Embodiment 6:

[0048] (1) Take 216 g of phosphotungstic acid aqueous solution (mass fraction 15 wt%), add 10.5 g of aminopropylmethyldiethoxysilane dropwise under magnetic stirring, react at 50° C. for 24 h, and then evaporate the water under reduced pressure to obtain a white powder.

[0049] (2) The white powder was added to a solution of 12.6 g of phenyl glycidyl ether and 110 g of toluene, and the temperature was raised to 70° C. under magnetic stirring and reflux for 5 h, then cooled to room temperature and dried under reduced pressure to obtain the product.

[0050] (3) Add 5% of the above solid powder into epoxy resin for curing.

[0051] Embodiment 7:

[0052] (1) Take 216 g of phosphotungstic acid aqueous solution (mass fraction 15 wt%), add 7.5 g of aminopropyltriethoxysilane dropwise under magnetic stirring, react at 60° C. for 20 h, and then evaporate the water under reduced pressure to obtain a white powder.

[0053] (2) The white powder was added to a solution of 6.3 g of octyl glycidyl ether and 700 g of xylene, and the temperature was raised to 70° C. under magnetic stirring and reflux, and the temperature was kept for 5 h, then the temperature was lowered to room temperature, and the product was dried under reduced pressure to obtain the product.

[0054] (3) Add 5% of the above solid powder into epoxy resin for curing.

[0055] Embodiment 8:

[0056] (1) 136 g of ethanol solution of phosphomolybdic acid (mass fraction 15 wt%) was added dropwise with 7.4 g of aminopropyltriethoxysilane under magnetic stirring, and the mixture was reacted at 60° C. for 24 h, and then the water was evaporated under reduced pressure to obtain a white powder.

[0057] (2) The above product was added to a solution of 5 g of phenyl glycidyl ether and 100 g of xylene, heated to 80° C. with magnetic stirring for 3 h, cooled to room temperature, and dried under reduced pressure to obtain the product.

[0058] (3) Add 5% of the above solid powder into epoxy resin for curing.

[0059] In order to more intuitively demonstrate the process advantages of the present invention, the preparation method of the heteropolyacid siloxane glycidyl ether composite material of the present invention is compared with the method of using equivalent replacement in the same process.

[0060] Comparative Example 1:

[0061] Same as Example 1, except that phosphotungstic acid is replaced by silicomolybdic acid;

[0062] (1) 136.7 g of silicomolybdic acid aqueous solution (mass fraction 15 wt%) was added dropwise with 10 g of aminopropyltriethoxysilane under magnetic stirring, and the mixture was reacted at 50° C. for 18 h. The water was evaporated under reduced pressure to obtain a white powder.

[0063] (2) The white powder was added to a solution of 11 g of octyl glycidyl ether and 135 g of xylene, and the temperature was raised to 85° C. with magnetic stirring and kept for 3 h, then cooled to room temperature and dried under reduced pressure to obtain the product.

[0064] (3) Add 5% of the above solid powder into epoxy resin for curing.

[0065] Comparative Example 2:

[0066] Same as Example 1, except that phosphotungstic acid is replaced with silicotungstic acid;

[0067] (1) Take 216 g of silicotungstic acid aqueous solution (mass fraction 15 wt%), add 10 g of aminopropyltriethoxysilane dropwise under magnetic stirring, react at 50° C. for 18 h, and then evaporate the water under reduced pressure to obtain a white powder.

[0068] (2) The white powder was added to a solution of 11 g of octyl glycidyl ether and 135 g of xylene, and the temperature was raised to 85° C. with magnetic stirring and kept for 3 h, then cooled to room temperature and dried under reduced pressure to obtain the product.

[0069] (3) Add 5% of the above solid powder into epoxy resin for curing.

[0070] Comparative Example 3:

[0071] Example 1: The difference is that the alkyl glycidyl ether is replaced by epichlorohydrin;

[0072] (1) Take 216 g of phosphotungstic acid aqueous solution (mass fraction 15 wt%), add 10 g of aminopropyltriethoxysilane dropwise under magnetic stirring, react at 50° C. for 18 h, and then evaporate the water under reduced pressure to obtain a white powder.

[0073] (2) The white powder was added to a solution of 11 g of epichlorohydrin and 135 g of xylene, and the temperature was raised to 85° C. with magnetic stirring and kept for 3 h, then cooled to room temperature and dried under reduced pressure to obtain the product.

[0074] (3) Add 5% of the above solid powder into epoxy resin for curing.

[0075] Comparative Example 4:

[0076] Same as Example 1, except that xylene is replaced by isopropanol;

[0077] (1) Take 216 g of phosphotungstic acid aqueous solution (mass fraction 15 wt%), add 10 g of aminopropyltriethoxysilane dropwise under magnetic stirring, react at 50° C. for 18 h, and then evaporate the water under reduced pressure to obtain a white powder.

[0078] (2) The white powder was added to a solution of 11 g of octyl glycidyl ether and 135 g of isopropanol, and the temperature was raised to 85° C. with magnetic stirring and kept for 3 h, then cooled to room temperature and dried under reduced pressure to obtain the product.

[0079] (3) Add 5% of the above solid powder into epoxy resin for curing.

[0080] Comparative Example 5:

[0081] Same as Example 1, except that the compounding effect of heteropolyacid siloxane glycidyl ether was not introduced;

[0082] (1) Take 216 g of phosphotungstic acid aqueous solution (mass fraction 15 wt%), add 10 g of aminopropyltriethoxysilane dropwise under magnetic stirring, react at 50° C. for 18 h, and then evaporate the water under reduced pressure to obtain a white powder.

[0083] (2) Add 5% of the above solid powder into epoxy resin for curing.

[0084] Comparative Example 6:

[0085] Same as Example 1, except that phosphotungstic acid is replaced by silicotungstic acid; alkane glycidyl ether is replaced by glycerol triglycidyl ether;

[0086] (1) Take 216 g of silicotungstic acid aqueous solution (mass fraction 15 wt%), add 10 g of aminopropyltriethoxysilane dropwise under magnetic stirring, react at 50° C. for 18 h, and then evaporate the water under reduced pressure to obtain a white powder.

[0087] (2) The white powder was added to a solution of 10 g of propylene glycol triglycidyl ether and 135 g of xylene, and the temperature was raised to 85° C. with magnetic stirring and kept for 3 h, then cooled to room temperature and dried under reduced pressure to obtain the product.

[0088] (3) Add 5% of the above solid powder into epoxy resin for curing.

[0089] The dispersibility of the product in epoxy resin was determined by visual inspection in HG / T 5606-2019. The thermal weight loss performance was tested by TG-DSC thermal weight loss instrument in air atmosphere from 100-1000°C with a heating rate of 10°C / min, and the heat resistance was tested by weight loss rate.

[0090] Table 1: Comparison of dispersibility and thermal weight loss performance of different embodiments and comparative examples:

[0091]

[0092] From the data analysis in Table 1, we can see that:

[0093] (1) Examples 1-9 have no significant differences in agglomeration and thermal weight loss performance; and have good compatibility with epoxy resin, and significantly improve heat resistance.

[0094] Taking Example 1 as an example, the infrared spectrum of the product of Example 1 is as follows Figure 1 As shown, the spectrum shows silicon oxygen bond (980cm-1), hydroxyl bond (3000-3200cm-1), and long chain alkane bond (1690cm-1, 1550cm-1), indicating the successful compounding of heteropolyacid siloxane glycidyl ether. The cured product was characterized by thermogravimetric properties, the test conditions were 100-800℃, the heating rate was 10℃ / min, and the heat resistance of the product was evaluated by thermogravimetric loss.

[0095] in, Figure 2 This is an optical photograph after adding epoxy resin component A to Example 1. The product of Example 1 is uniformly dispersed in the epoxy resin. Figure 4 The thermogravimetric spectra of pure epoxy resin and the product of Example 1 are shown. It can be seen that the epoxy resin with the product of Example 1 has a thermal weight loss of 12% at 300°C, while the pure epoxy resin has a thermal weight loss of 20% at 300°C. After adding the product of Example 1, the thermal decomposition temperature and heat resistance of the epoxy resin are significantly improved. The product of Example 1 is well dispersed in the epoxy resin, and the contact area between the two is greatly increased, which effectively improves its heat resistance.

[0096] This may be because the present invention firstly utilizes the hydrolysis and polycondensation reaction of the aminosilane coupling agent to graft the silane alkoxy group into the structure of the heteropoly acid, forming a chemical combination between the surface of the heteropoly acid and the silanol group, forming a surface organic silicon coating, and improving the performance of the heteropoly acid as a heat-resistant additive. In order to improve the compatibility and dispersibility with the epoxy resin, the heteropoly acid siloxane is further reacted with phenyl glycidyl ether or octyl glycidyl ether, and the epoxy group in the glycidyl ether is further reacted with the amino group in the above product, and the phenyl glycidyl ether or octyl glycidyl ether is further modified to further improve the heat resistance.

[0097] (2) Comparative Examples 1 and 2 show good compatibility with epoxy resin and no obvious agglomeration. However, the thermal weight loss performance is poor. The thermal weight loss of the product of Comparative Example 1 added to epoxy resin at 300°C is 18%, which is much lower than 12% of the present invention.

[0098] This shows that the type of heteropoly acid is an influencing factor of the compatibility of epoxy resin. Among them, the heteropoly acid that is a phosphotungstic acid aqueous solution or a phosphomolybdic acid ethanol solution can have a more positive effect on the compatibility of epoxy resin, while other heteropoly acids have no positive effect.

[0099] (3) From the experimental data of Comparative Examples 3 and 5,

[0100] Comparative Example 3 differs from Example 1 in that the alkyl glycidyl ether is replaced with epichlorohydrin in order to introduce epoxy groups;

[0101] Comparative Example 5 is different from Example 1 in that no heteropolyacid siloxane glycidyl ether is introduced, and does not have the composite effect of heteropolyacid siloxane glycidyl ether;

[0102] According to the experimental results, there is no difference in the heat resistance of Example 3 and Example 5. The experimental results show that Figure 3 This is an optical photograph of comparative example 3 after adding epoxy resin component A. The product of comparative example 3 has serious particle agglomeration in the epoxy resin. It can be seen that conventional glycidyl ether or epoxy group epichlorohydrin does not have a positive effect on the heat resistance of epoxy resin, and has poor compatibility with epoxy resin, resulting in serious agglomeration problems;

[0103] (4) According to the experimental data from Example 4,

[0104] Comparative Example 4 is different from Example 1 in that the solvent is isopropanol, which causes the heat resistance of the epoxy resin to deteriorate and also causes serious agglomeration problems. It can be seen that the solvent xylene or toluene also has a positive effect on the heat resistance of the epoxy resin.

[0105] (6) According to the experimental data from Example 6,

[0106] Comparative Example 6 is different from Example 1 in that phosphotungstic acid is replaced by silicotungstic acid; alkane glycidyl ether is replaced by glycerol triglycidyl ether;

[0107] According to the experimental results, the comparative example did not have the agglomeration problem, but the heat resistance was deteriorated. Therefore, it can be seen that propylene glycol triglycidyl ether can alleviate the agglomeration problem, but has no positive effect on the heat resistance.

[0108] In summary: the present invention firstly utilizes the hydrolysis and polycondensation reaction of the aminosilane coupling agent to graft the silane alkoxy group into the structure of the heteropoly acid, thereby forming a chemical combination between the surface of the heteropoly acid and the silanol group, forming a surface organic silicon coating, and improving the performance of the heteropoly acid as a heat-resistant additive. In order to improve the compatibility and dispersibility with the epoxy resin, the heteropoly acid siloxane is further reacted with phenyl glycidyl ether or octyl glycidyl ether, and the epoxy group in the glycidyl ether is further reacted with the amino group in the above product, and the phenyl glycidyl ether or octyl glycidyl ether is further modified to further improve the heat resistance.

Claims

1. A method for preparing a heteropolyacid siloxane glycidyl ether composite material, characterized in that: The preparation of the heteropolyacid siloxane glycidyl ether composite material comprises the following steps: (1) dispersing a heteropoly acid in a solvent of xylene or toluene, adding an aminosilane coupling agent dropwise, distilling under reduced pressure after the reaction, and drying to obtain a solid product; the heteropoly acid is a phosphotungstic acid aqueous solution or a phosphomolybdic acid ethanol solution; (2) The solid powder is dispersed in a solution of alkyl glycidyl ether, reacted at a certain temperature, and then distilled under reduced pressure and dried to obtain a product.

2. The method for preparing the heteropolyacid siloxane glycidyl ether composite material according to claim 1, characterized in that In step (1), the mass fraction of the phosphotungstic acid aqueous solution is 5-20wt%; the mass fraction of the phosphomolybdic acid ethanol solution is 5-20wt%.

3. The method for preparing the heteropolyacid siloxane glycidyl ether composite material according to claim 1, characterized in that In step (1), the aminosilane coupling agent is any one of aminopropyltrimethoxysilane, aminopropyltriethoxysilane, aminopropylmethyldimethoxysilane and aminopropylmethyldiethoxysilane.

4. The method for preparing the heteropolyacid siloxane glycidyl ether composite material according to claim 1, characterized in that In step (1), the reaction temperature is 40-60°C and the reaction time is 12-24h.

5. The method for preparing the heteropolyacid siloxane glycidyl ether composite material according to claim 1, characterized in that The molar ratio of the heteropoly acid to the aminosilane coupling agent is 1:(3-5).

6. The method for preparing the heteropolyacid siloxane glycidyl ether composite material according to claim 1, characterized in that In step (2), the alkane glycidyl ether is phenyl glycidyl ether or octyl glycidyl ether.

7. The method for preparing the heteropolyacid siloxane glycidyl ether composite material according to claim 1, characterized in that In step (2), the mass fraction of the alkyl glycidyl ether solution is 5-10wt%, and the molar number of the alkyl glycidyl ether is 1-1.5 times that of the aminosilane coupling agent.

8. The method for preparing the heteropolyacid siloxane glycidyl ether composite material according to claim 1, characterized in that In step (2), the reaction temperature is 70-100° C. and the reaction time is 2-5 h.

9. A heteropolyacid siloxane glycidyl ether composite material, prepared by the preparation method of the heteropolyacid siloxane glycidyl ether composite material according to any one of claims 1 to 8, characterized in that The heteropolyacid siloxane glycidyl ether composite material is used as an epoxy resin heat resistant agent.

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