Preparation method of multi-level interface regulation and control type high-strength composite material

Abstract

The invention relates to the technical field of polymer composite materials, and particularly discloses a preparation method of a multistage interface regulation and control type high-strength composite material. The preparation method comprises the following steps: treating graphene oxide with a silane coupling agent KH-550, grafting with carbon nanotubes, and modifying with isocyanate to obtain a modified carbon hybrid filler; and mixing the modified carbon hybrid filler with caprolactam, and inducing the molecular chain of polyamide 6 to grow along the chain on the surface of the filler, thereby preparing the graphene oxide grafted carbon nanotube reinforced polyamide 6 composite material. Through the two strong interfaces, the internal stress transmission efficiency of the interface can be improved, the thermal resistance of the interface can be reduced, the tensile strength and the heat-conducting property of the polymer are remarkably improved, and the problems of low tensile strength and poor heat-conducting property of the polymer are effectively solved.

Description

Technical Field

[0001] The present invention relates to the technical field of polymer composites, and particularly relates to a preparation method of a multi-level interface-regulated high-strength composite material. Background Art

[0002] As the most potential clean energy carrier in the 21st century, the large-scale application of hydrogen energy depends on safe and efficient storage and transportation technologies. On-vehicle high-pressure gaseous hydrogen storage technology has become the mainstream due to its simple equipment structure and high charging and discharging efficiency. Among them, type-IV hydrogen storage cylinders have become the core energy storage equipment for hydrogen fuel cell vehicles due to the advantages of lightweight, hydrogen embrittlement resistance, and high hydrogen storage density of non-metallic inner liners and fully wound carbon fiber structures. However, its large-scale industrialization still faces multiple technical bottlenecks. Among them, ensuring the high strength and high thermal conductivity of the inner liner material of type-IV hydrogen storage cylinders is one of the core indicators to ensure its safe and efficient operation.

[0003] During the rapid charging and discharging of hydrogen, the thermo-mechanical coupling effect has a decisive impact on the structural integrity and gas barrier performance of the polymer inner liner. Mechanically, the transient hydrogen pressure fluctuation causes dynamic deformation of the polymer lining. If the material strength is insufficient, it is easy to fail under cyclic pressurization conditions. Thermally, the Joule-Thomson effect generates a sharp temperature gradient. If the thermal conductivity of the material is low, uneven heat conduction will generate local thermal stress. The long-term action of stress concentration may induce the generation and propagation of microcracks, resulting in a decrease in the mechanical properties and hydrogen gas barrier performance of the material, and reducing the safety of the hydrogen storage system. Therefore, by adding nano-fillers (such as graphene oxide, carbon nanotubes) to polymer materials and developing high-strength and high-thermal conductivity modified polymers, the problem of inner liner failure caused by thermo-mechanical coupling can be effectively solved, thereby improving the service life of hydrogen storage cylinders.

[0004] However, the current methods for adding nano-fillers are mainly based on blending processes. There are mostly weak interfacial connections between fillers and between fillers and the polymer matrix, reducing the interfacial stress transfer efficiency and having a large interfacial thermal resistance, resulting in the insufficient utilization of the excellent mechanical and thermal properties of the fillers. Therefore, how to construct strong interfaces between fillers / fillers and fillers / polymer matrices and prepare multi-level interface-regulated high-strength composite materials to effectively solve the problem of failure caused by thermo-mechanical coupling of polymer inner liners is the key problem that needs to be solved urgently for current polymer inner liner materials. Summary of the Invention

[0005] In order to make up for the deficiencies of the prior art, the present invention provides a preparation method of a multi-level interface-regulated high-strength composite material based on strong interfaces between fillers / fillers and fillers / matrix.

[0006] The present invention is realized by the following technical solutions: A preparation method of a multi-level interface-regulated high-strength composite material includes the following steps: S1. Mix graphene oxide, 1-ethyl-(3-dimethylaminopropyl)carbodiimide hydrochloride, 1-hydroxybenzotriazole monohydrate, and N,N'-diisopropylethylamine. After magnetic stirring evenly, add silane coupling agent KH-550 (γ-aminopropyltriethoxysilane). Fill the reaction device with nitrogen, reflux and stir at 60 °C for 24 h, and then filter to obtain functionalized graphene oxide. S2. Mix and disperse functionalized graphene oxide and hydroxylated multi-walled carbon nanotubes, then add glacial acetic acid to adjust the pH, and heat to reflux for reaction to achieve grafting of graphene oxide and carbon nanotubes. S3. After dispersing the obtained grafting product evenly, add isocyanate and catalyst, and react at 40 - 80 °C under nitrogen atmosphere for 0.5 - 3 h to obtain isocyanate-modified carbon hybrid filler. S4. Melt caprolactam and add the above-obtained carbon hybrid filler dispersion liquid. Remove the dispersion solvent, then add sodium hydroxide. After heating to 135 °C, add TDI (toluene diisocyanate), stir evenly, then cast it into a preheated mold, keep warm and then naturally cool and demold to obtain a composite material. Cut the composite material into small particles and boil in water to remove unreacted monomers to obtain the product.

[0007] In this invention, graphene oxide is first treated with silane coupling agent KH-550 (γ-aminopropyltriethoxysilane), then grafted with carbon nanotubes, and then modified with isocyanate to obtain modified carbon hybrid filler; mix the modified carbon hybrid filler with caprolactam to induce chain growth of polyamide 6 molecular chains along the surface of the filler, thereby preparing a polyamide 6 composite material reinforced by graphene oxide grafted carbon nanotubes.

[0008] In this invention, the coupling agent realizes strong covalent bonding between graphene oxide and carbon nanotubes, and then strong covalent bonding between the filler and the polyamide 6 matrix is realized through isocyanate modification of the filler. The prepared composite material has excellent tensile strength and thermal conductivity.

[0009] A more preferred technical solution of this invention is as follows: In step S1, the surface of graphene oxide contains hydroxyl and carboxyl functional groups. Disperse graphene oxide in DMF (N,N-dimethylformamide) by ultrasonic treatment, then add 1-ethyl-(3-dimethylaminopropyl)carbodiimide hydrochloride, 1-hydroxybenzotriazole monohydrate, and N,N'-diisopropylethylamine, stir evenly by magnetic force, and dropwise add silane coupling agent KH-550 (γ-aminopropyltriethoxysilane) into the suspension.

[0010] Further preferably, wash the obtained functionalized graphene oxide by filtration successively with water, absolute ethanol, and DMF for several times and reserve for use.

[0011] In step S2, functionalized graphene oxide and hydroxylated multi-walled carbon nanotubes are ultrasonically dispersed in DMF / deionized water for 12 - 18 min. Then, glacial acetic acid is added to the reaction solution to adjust the pH value to 3 - 4, and the reaction is refluxed at 60 °C for 24 h. Among them, only hydroxyl functional groups exist on the surface of the carbon nanotubes.

[0012] More preferably, after the grafting reaction is completed, the suction filtration product is washed several times with absolute ethanol, deionized water, and DMF to remove by-products, and a carbon hybrid filler is obtained.

[0013] In step S3, the grafted product is ultrasonically dispersed in anhydrous DMF for 8 - 12 min. Then, isocyanate and a catalyst are added, and the reaction is carried out at 60 °C under a nitrogen atmosphere for 1 h. After the reaction is completed, the product is suction filtered with DMF repeatedly for 2 - 3 times, and the isocyanate-modified carbon hybrid filler obtained is dispersed in anhydrous DMF.

[0014] More preferably, the isocyanate is toluene diisocyanate, isophorone diisocyanate, hexamethylene diisocyanate, hexamethylene diisocyanate trimer, dicyclohexylmethane diisocyanate, diphenylmethane diisocyanate, or lysine diisocyanate; and the catalyst is an organotin compound.

[0015] In step S4, caprolactam is melted at 80 °C and then added to the carbon hybrid filler dispersion liquid. The dispersion solvent DMF is removed by distillation. Then, sodium hydroxide is added, and the mixture is heated in an oil bath at 135 °C under high vacuum. Toluene diisocyanate (TDI) is added and stirred evenly. It is quickly cast into a preheated mold, and after heat preservation, it is naturally cooled and demolded to obtain a composite material. The composite material is cut into small particles and boiled in water to remove unreacted monomers to obtain the product.

[0016] More preferably, the method for removing the dispersion solvent is simple distillation or vacuum distillation; the temperature of the preheated mold is 145 - 180 °C, and the heat preservation time is 10 - 180 min.

[0017] The present invention first realizes the chemical bonding between graphene oxide and carbon nanotubes through a coupling agent, constructing a strong interfacial bond between the filler and the filler part. Then, through surface isocyanate modification of the carbon hybrid filler, the chemical bonding between the polymer molecular chain and the filler surface is realized, constructing a strong interfacial bond between the filler and the matrix.

[0018] Through the two strong interfaces constructed above, the present invention can improve the interfacial internal stress transfer efficiency, reduce the interfacial thermal resistance, significantly improve the tensile strength and thermal conductivity of the polymer, and effectively solve the problems of low tensile strength and poor thermal conductivity of the polymer. BRIEF DESCRIPTION OF THE DRAWINGS

[0019] The present invention will be further described below with reference to the accompanying drawings.

[0020] Figure 1 Transmission electron microscopy morphology of graphene oxide grafted carbon nanotubes; Figure 2 Thermal conductivity comparison of composites with different filler concentrations. Specific embodiments

[0021] To make the above objects, features, and advantages of the present invention more obvious and understandable, the following describes the specific embodiments of the present invention in detail with reference to the accompanying drawings. Many specific details are set forth in the following description to facilitate a thorough understanding of the present invention. However, the present invention can be implemented in many other ways different from those described herein, and those skilled in the art can make similar improvements without departing from the connotation of the present invention. Therefore, the present invention is not limited by the specific embodiments disclosed below.

[0022] Example 1: A preparation method of a multi-level interface-regulated high-strength composite material First, this example provides a chemical grafting method of graphene oxide and carbon nanotubes, including the following steps: S1. Functionalize graphene oxide by the carbodiimide method First, take 200 mg of graphene oxide and ultrasonically disperse it in 50 ml of DMF for 15 min. Add 80 mg of 1-ethyl-(3-dimethylaminopropyl)carbodiimide hydrochloride, 80 mg of 1-hydroxybenzotriazole monohydrate, and 1.2 ml of N,N'-diisopropylethylamine, and stir magnetically until evenly mixed. Subsequently, gradually add 400 mg of silane coupling agent KH-550 dropwise to the suspension, fill the reaction device with nitrogen, and reflux and stir the reaction at 60 °C for 24 h. Finally, obtain functionalized graphene oxide by filtration, wash the reaction product several times with deionized water, absolute ethanol, and DMF to remove the unreacted silane coupling agent KH-550 and other by-products, and reserve it for use.

[0023] The purpose of step S1 is to induce the reaction between the amino group on the silane coupling agent KH-550 and the carboxyl group on graphene oxide, realizing the chemical grafting of one end of the silane coupling agent KH-550 and graphene oxide; the excessive amino silane is to fully consume the carboxyl group on graphene oxide to prevent the carboxyl group from participating in the reaction and causing chain termination when the subsequent filler and polymer molecule are grafted, resulting in a decrease in the polymer molecular weight.

[0024] S2. Ultrasonically disperse 100 mg of silane coupling agent KH-550 functionalized graphene oxide and 80 mg of hydroxylated multi-walled carbon nanotubes in 100 ml of DMF (volume ratio 9:1) for 15 min; then, add a certain amount of glacial acetic acid to the reaction solution to maintain the pH value of the reaction solution at 3.5 ± 0.1. At this pH value, the mixture is refluxed at 60 °C for 16 h to achieve the grafting of graphene oxide and carbon nanotubes; after the reaction is completed, wash the suction filtration product several times with absolute ethanol, deionized water and DMF to remove by-products and obtain the carbon hybrid filler.

[0025] The purpose of step S2 is to induce the reaction between the siloxy groups on the silane coupling agent KH-550 and the hydroxyl groups on the multi-walled carbon nanotubes, realize the chemical grafting of the functional groups at the other end of the silane coupling agent KH-550 and the carbon nanotubes, and finally make the two ends of the silane coupling agent KH-550 connect graphene oxide and carbon nanotubes respectively, realizing a strong interfacial bond between graphene oxide and carbon nanotubes. The purpose of adding deionized water is to promote the hydrolysis of the siloxy groups in the amino silane, thus accelerating the grafting reaction; the purpose of maintaining the pH value at 3.5 ± 0.1 is to inhibit the homocondensation of the siloxy groups.

[0026] In the second aspect, this embodiment provides a method for in-situ polymerization to prepare a carbon hybrid filler reinforced polyamide 6 composite material, including the following steps: S3. Before the experiment, treat DMF with molecular sieves to remove moisture Ultrasonically disperse 100 mg of the grafting product in 100 ml of DMF for 10 min, add 3 g of HDI (hexamethylene diisocyanate), and stir evenly; then add 50 mg of dibutyltin dilaurate and react at 60 °C under a nitrogen atmosphere for 1 h; after the reaction is completed, repeatedly filter the modified graphene oxide grafted carbon nanotubes with DMF 3 times to remove unreacted HDI and other by-products; disperse the obtained clean product in anhydrous DMF for the synthesis of the composite material.

[0027] The purpose of step S3 is to introduce highly reactive isocyanate groups on the surface of the graphene oxide grafted carbon nanotube hybrid filler; the purpose of adding dibutyltin dilaurate is to accelerate the reaction between the hydroxyl groups on the filler and the isocyanate groups.

[0028] In this step, HDI, that is, hexamethylene diisocyanate, is used to modify the nano filler to achieve the isocyanate modification of the surface of the carbon hybrid filler. HDI is a diisocyanate with an isocyanate group at each end. One of the groups can react with the hydroxyl groups on the filler, and after the reaction, a part of the unreacted isocyanate groups (the functional groups at the other end) will be retained, and the unreacted isocyanate groups can participate in the in-situ polymerization reaction of polyamide 6.

[0029] When modifying the filler, the main purpose is to introduce isocyanate groups. Isocyanate groups are highly reactive and will react with the hydroxyl groups on the filler. Therefore, diisocyanates are used, such as those mentioned earlier: toluene diisocyanate, isophorone diisocyanate, hexamethylene diisocyanate, hexamethylene diisocyanate trimer, dicyclohexylmethane diisocyanate, diphenylmethane diisocyanate or lysine diisocyanate. The purpose is to retain some isocyanate groups so that the filler can participate in the polymerization process of the polymer.

[0030] Organotin catalysts are relatively commonly used catalysts. In addition to dibutyltin dilaurate, stannous octoate can also be used. The difference is that different tin-based catalysts have different catalytic speeds.

[0031] S4. Before the experiment, caprolactam and sodium hydroxide are dried. First, place 20 g of caprolactam in a three-necked flask. After melting at 80 °C, add a certain amount of DMF dispersion of carbon hybrid filler, and use the method of vacuum distillation to remove DMF from the reaction system. Then, add 30 mg of sodium hydroxide, heat it in an oil bath to 135 °C. At this temperature, promote the formation of caprolactam anionic polymerization for chain growth between sodium hydroxide and caprolactam. During this period, the reaction device is kept in a high vacuum state. Finally, add 115 mg of TDI (toluene diisocyanate), stir evenly, and quickly cast it into a preheated mold in a 160 °C vacuum oven, and keep it warm for 50 min. Wait for it to cool naturally and demold. Cut the composite material into small particles, boil it in boiling water for 3 h to remove unreacted monomers, and finally obtain the product.

[0032] The purpose of step S4 is to induce the chain growth of polyamide 6 molecular chains on the surface of the hybrid filler, so as to achieve a strong interfacial bond between the filler and the polymer matrix. The purpose of drying the raw materials before the experiment and keeping the device in a high vacuum state during the reaction is to remove trace moisture in the raw materials and the reaction system, because moisture is an inhibitor for the polymerization of polyamide 6.

[0033] In the process of synthesizing polyamide 6, isocyanate is also needed. Toluene diisocyanate (TDI) is used. This isocyanate is used as a reaction activator to lower the reaction temperature. If it is not added, the reaction requires a temperature above 200 °C, but after adding, the reaction can occur at 160 °C. The isocyanate group on TDI plays a role in activating the reaction and reducing the reaction activation energy.

[0034] Example 2: A preparation method of a multi-level interface-regulated high-strength composite material The specific steps and principles of this example are as in Example 1. The main difference from Example 1 is: In step S2, functionalized graphene oxide and hydroxylated multi-walled carbon nanotubes are placed in DMF / deionized water and ultrasonically dispersed for 12 min. Then, glacial acetic acid is added to the reaction solution to adjust the pH value to 3 ± 0.1; In step S3, 100 mg of the grafted product is ultrasonically dispersed in 100 ml of anhydrous DMF for 8 min. Then, 5 g of toluene diisocyanate and 50 mg of stannous octoate catalyst are added, and the reaction is carried out at a temperature of 40 °C in a nitrogen atmosphere for 3 h; after the reaction is completed, the product is repeatedly filtered with DMF twice, and the obtained isocyanate-modified carbon hybrid filler is dispersed in anhydrous DMF; In step S4, the method for removing the dispersion solvent is simple distillation; the temperature for preheating the mold is 145 °C, and the heat preservation time is 180 min.

[0035] Example 3: A preparation method of a multi-level interface-regulated high-strength composite material The specific steps and principles of this example are as in Example 1. The main difference from Example 1 is as follows: In step S2, functionalized graphene oxide and hydroxylated multi-walled carbon nanotubes are placed in DMF / deionized water and ultrasonically dispersed for 18 min. Then, glacial acetic acid is added to the reaction solution to adjust the pH value to 4 ± 0.1; In step S3, 100 mg of the grafted product is ultrasonically dispersed in 100 ml of anhydrous DMF for 12 min. Then, 4 g of hexamethylene diisocyanate trimer and 50 mg of stannous octoate catalyst are added, and the reaction is carried out at a temperature of 80 °C in a nitrogen atmosphere for 0.5 h; In step S4, the temperature for preheating the mold is 180 °C, and the heat preservation time is 30 min.

[0036] As shown in the appendix Figure 1 It can be seen that through the grafting process of the present invention, the connection of the two ends of the carbon nanotubes with different graphene oxide sheets is realized, and the construction of the chemical bond grafting path between different sheets is realized.

[0037] As can be seen from the following table, the hybrid filler system has better tensile strength than the single filler system, indicating that the hybridization of graphene oxide and carbon nanotubes to enhance polyamide 6 has a synergistic effect; the tensile strength of the isocyanate-modified carbon hybrid filler-enhanced polyamide 6 is more excellent than that of the unmodified hybrid filler system, reflecting the modification effect. The specific effects are as follows.

[0038] As shown in the appendix Figure 2 It can be seen that the isocyanate-modified carbon hybrid filler-enhanced polyamide 6 has the highest thermal conductivity coefficient, reflecting the advantage of constructing two strong interfaces.

[0039] The development of hydrogen energy has put forward stringent requirements for the mechanical properties and thermal conductivity of polyamide 6 (PA6) liner materials for hydrogen storage cylinders. However, the weak interfacial bonding in PA6 composites makes it difficult for the excellent mechanical and thermal properties of the reinforcing phase to be efficiently transferred through the interface. In this invention, hexamethylene diisocyanate (HDI) is used to covalently suture hydroxylated carbon nanotubes (CNT-OH) hybrid fillers with graphene oxide (GO) to construct nano-hybrid fillers (fGO+CNT-OH+HDI) with active isocyanate groups on the surface. Taking this as an activator to participate in the in-situ anionic polymerization reaction of caprolactam, the preparation of PA6 composites based on strong interfaces of filler / filler and filler / matrix is thus realized.

[0040] Combined with the synergistic strengthening effect of the hybrid fillers and the uniform dispersion characteristics brought by in-situ polymerization, the PA6 composite containing only 0.2 wt% fGO+CNT-OH+HDI shows high strength-high toughness characteristics, including a 36.3% increase in tensile strength and an ultra-high fracture strain of 130.86%; in addition, the thermal conductivity of the composite also increases by 46.3%. This interfacial strengthening strategy breaks through the performance bottleneck of traditional composites, can effectively improve the use reliability and safety of hydrogen storage cylinders, and provides key material support for the efficient storage, transportation and large-scale application of the hydrogen energy industry.

[0041] Finally, it should be noted that the above embodiments are only used to illustrate the technical solutions of the present invention, rather than to limit them; although the present invention has been described in detail with reference to the foregoing embodiments, those of ordinary skill in the art should understand that: they can still modify the technical solutions recorded in the foregoing embodiments, or perform equivalent replacements on some or all of the technical features; and these modifications or replacements do not make the essence of the corresponding technical solutions deviate from the scope of the technical solutions of the embodiments of the present invention, and they should all be covered by the scope of the claims and the specification of the present invention.

Claims

1. A preparation method of a multi-level interface regulation type high-strength composite material, characterized in that, It includes the following steps: S1. Graphene oxide, 1-ethyl-(3-dimethylaminopropyl)carbodiimide hydrochloride, 1-hydroxybenzotriazole monohydrate, and N,N'-diisopropylethylamine are mixed. After magnetic stirring evenly, silane coupling agent KH-550 is added. The reaction device is filled with nitrogen, and reflux stirring reaction is carried out at 60 °C for 24 h, and then suction filtration is carried out to obtain functionalized graphene oxide; S2. Functionalized graphene oxide and hydroxylated multi-walled carbon nanotubes are mixed and dispersed, and then glacial acetic acid is added to adjust the pH, and the temperature is raised for reflux reaction to achieve grafting of graphene oxide and carbon nanotubes; S3. After the obtained grafted product is dispersed evenly, isocyanate and a catalyst are added, and reaction is carried out at a temperature of 40-80 °C and in a nitrogen atmosphere for 0.5-3 h to obtain isocyanate-modified carbon hybrid filler; S4. Caprolactam is melted and then the above-obtained carbon hybrid filler dispersion liquid is added, the dispersion solvent is removed, and then sodium hydroxide is added. After the temperature is raised to 135 °C, toluene diisocyanate is added. After stirring evenly, it is cast into a preheated mold, and after heat preservation, it is naturally cooled and demolded to obtain a composite material. The composite material is cut into small particles and boiled in water to remove unreacted monomers to obtain the product.

2. The preparation method of the multi-level interface regulation type high-strength composite material according to claim 1, characterized in that: In step S1, the surface of graphene oxide contains hydroxyl and carboxyl functional groups. Graphene oxide is placed in DMF and ultrasonically dispersed, and then 1-ethyl-(3-dimethylaminopropyl)carbodiimide hydrochloride, 1-hydroxybenzotriazole monohydrate, and N,N'-diisopropylethylamine are added. After magnetic stirring evenly, KH-550 is added dropwise to the suspension.

3. The preparation method of the multi-level interface regulation type high-strength composite material according to claim 2, characterized in that: The obtained functionalized graphene oxide by suction filtration is washed several times with water, absolute ethanol, and DMF in sequence and reserved for use.

4. The preparation method of the multi-level interface regulation type high-strength composite material according to claim 1, wherein: In step S2, functionalized graphene oxide and hydroxylated multi-walled carbon nanotubes are placed in DMF / deionized water and ultrasonically dispersed for 12-18 min. Then, glacial acetic acid is added to the reaction solution to adjust the pH value to 3-4, and reflux reaction is carried out at 60 °C for 24 h; among them, only hydroxyl functional groups exist on the surface of the carbon nanotubes.

5. The preparation method of the multi-level interface regulation type high-strength composite material according to claim 4, characterized in that: After the grafting reaction is completed, the suction filtration product is washed several times with absolute ethanol, deionized water, and DMF to remove by-products to obtain carbon hybrid filler.

6. The preparation method of the multi-level interface regulation type high-strength composite material according to claim 1, wherein: In step S3, the grafted product is ultrasonically dispersed in anhydrous DMF for 8-12 min, and then isocyanate and a catalyst are added, and reaction is carried out at a temperature of 60 °C and in a nitrogen atmosphere for 1 h; after the reaction is completed, the product is repeatedly suction filtered 2-3 times with DMF, and the obtained isocyanate-modified carbon hybrid filler is dispersed in anhydrous DMF.

7. The preparation method of the multi-level interface regulation type high-strength composite material according to claim 1 or 6, characterized in that: The isocyanate is toluene diisocyanate, isophorone diisocyanate, hexamethylene diisocyanate, hexamethylene diisocyanate trimer, dicyclohexylmethane diisocyanate, diphenylmethane diisocyanate, or lysine diisocyanate; the catalyst is an organotin compound.

8. The preparation method of the multi-level interface regulation type high-strength composite material according to claim 1, wherein: In step S4, caprolactam is melted at 80°C and then added to the carbon hybrid filler dispersion. The dispersion solvent DMF is removed by distillation. Then sodium hydroxide is added, and the mixture is heated to 135°C in an oil bath under high vacuum. Toluene diisocyanate is added and stirred evenly. It is quickly cast into a preheated mold, and after heat preservation, it is naturally cooled and demolded to obtain a composite material. The composite material is cut into small particles and boiled in water to remove unreacted monomers to obtain the product.

9. The preparation method of the multi-level interface regulation type high-strength composite material according to claim 1 or 8, characterized in that: In step S4, the method for removing the dispersion solvent is simple distillation or vacuum distillation; the temperature of the preheated mold is 145-180°C, and the heat preservation time is 10-180 min.

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