High-elasticity composite polymer material and preparation process therefor

Abstract

The present invention relates to the technical field of polymer materials, and in particular to a high-elasticity composite polymer material and a preparation process therefor. The present invention solves the problems of poor tensile strength, low impact strength, poor elastic properties, low aging resistance, and poor heat resistance of high-elasticity composite polymer materials. In the present invention, the high-elasticity composite polymer material is prepared from modified polyurethane, a modified rubber, a toughening agent, and modified inorganic particles by means of melt extrusion. In the present invention, the tensile properties of the composite material are improved by controlling the type and dosage of diisocyanate; the elastic properties of the composite material prepared by adjusting the dosages of the modified polyurethane and the modified rubber are improved; the impact strength of the composite material is improved by adjusting the type and dosage of the toughening agent; the aging resistance of the material is improved by introducing an ultraviolet absorber as an end-capping agent into the main body of the composite material; and the heat resistance of the composite material is improved by using nanoparticles modified with KH-792.

Description

A highly elastic composite polymer material and its preparation process Technical Field

[0001] This invention relates to the field of polymer materials technology, specifically to a highly elastic composite polymer material and its preparation process. Background Technology

[0002] Due to their unique physical and chemical properties, polymer materials are widely used in engineering, giving functional materials many excellent properties, such as high elasticity, wear resistance, shock resistance, and temperature resistance, or structural materials with certain special functions. Among them, rubber foam materials are polymer materials that combine the properties of rubber and foam materials. They constitute the viscoelasticity of rubber. Therefore, the characteristics of high-quality rubber are that it has both high elasticity and viscosity. It is often achieved by compounding multiple polymer materials to meet its performance requirements.

[0003] Patent CN104893015B reports a highly elastic rubber elastomer granule, which is composed of a rubber composition consisting of natural rubber, isoprene rubber, butadiene rubber, and ethylene-vinyl acetate copolymer, and then 1-4 parts of reinforcing agent, softener, plasticizer, crosslinking agent and other additives are added. The resulting rubber elastomer has high elasticity, high plasticity and low temperature resistance. However, the addition of the rubber composition reduces the anti-aging properties of the rubber elastomer and reduces its service life.

[0004] Patent CN104558513A discloses a melt reaction preparation method for nylon polyurethane elastomers. The method involves uniformly mixing amino-terminated nylon, isocyanate-terminated polyurethane, heat stabilizer, light stabilizer, and water stabilizer, and then carrying out a melt reaction using a twin-screw extruder or internal mixer. The nylon polyurethane elastomers prepared by this method have improved elasticity and the method is simple. However, the tensile strength is less than 30 MPa, and the mechanical properties need to be further improved.

[0005] Patent CN113337916B reports a method for dyeing spandex with reactive dyes. By introducing dihydroxy polymers containing tertiary amine groups into the soft segments of polyurethane elastic fibers and adding lithium organic compounds to the spinning aids of polyurethane elastic fibers, the dyeing rate of reactive dyes on polyurethane elastic fibers is improved, thereby enhancing the overall performance of the polymer material. However, the elastic properties of the polyurethane fibers prepared by this method are significantly altered, and the added lithium compounds accelerate the deterioration of the polyurethane elasticity, resulting in a reduction in the elastic properties of the material with long-term use.

[0006] Rubber materials refer to highly elastic polymer materials with reversible deformation. They are elastic at room temperature, capable of large deformation under small external forces, and return to their original shape after the force is removed. Therefore, the elastic properties of rubber products are widely used in various aspects of industry and daily life. Rubber is divided into natural rubber and synthetic rubber. Natural rubber is made by extracting latex from plants such as rubber trees and rubber grass. Natural rubber has good wear resistance, high elasticity, good tensile strength and elongation, and high resistance to acids and alkalis, but it still has problems such as poor heat resistance and easy aging in air.

[0007] Patent CN113278290B reports a high-temperature resistant silicone rubber and its preparation method. The silicone rubber prepared by methyl vinyl polysiloxane, silica, hydroxyl silicone oil, heat resistant agent and bis(2,4)-tetrachlorohydrin has high high-temperature resistance. However, the metal oxide can only keep the silicone rubber stable at around 200°C and it is difficult to withstand higher temperatures. In addition, the metal oxide has poor compatibility with the silicone rubber matrix, which further affects the mechanical properties of the silicone rubber.

[0008] In summary, existing technologies aim to achieve a synergistic increase in elasticity and mechanical properties by modifying polymer materials. However, the resulting composite polymer materials still suffer from poor elasticity, insufficient overall mechanical properties, and inadequate aging and heat resistance.

[0009] To this end, a highly elastic composite polymer material and its preparation process are proposed. Summary of the Invention

[0010] The present invention aims to provide a highly elastic composite polymer material and its preparation process. Modified polyurethane is prepared by condensing diisocyanate with polysiloxane, chain extension with polyethylene glycol, and end-capping with an end-capping agent. Silicone rubber and toughening rubber are polymerized using diisocyanate, and a reinforcing agent is added to the resulting mixed rubber, followed by vulcanization to obtain modified rubber. The modified polyurethane and modified rubber are melt-extruded to obtain the highly elastic composite polymer material. The tensile properties of the composite material are enhanced by changing the type and amount of diisocyanate and the average molecular weight of polyethylene glycol. Elastic properties are increased by using carbon nanotubes as a reinforcing agent and controlling the amount of modified polyurethane and modified rubber. Impact strength is improved by adjusting the type and amount of toughening agent. Anti-aging properties are improved by introducing ultraviolet absorbers into the main chain of the material by changing the amount of end-capping agent and modified polyurethane. The heat resistance of the material is improved by using KH-792 modified nano-titanium dioxide.

[0011] To achieve the above objectives, the present invention provides the following technical solution:

[0012] This invention provides a preparation process for a highly elastic composite polymer material, the preparation of which includes the following steps:

[0013] 60-120 parts of modified polyurethane, 40-70 parts of modified rubber, 5 parts of lubricant, 5 parts of antioxidant, 5-18 parts of toughening agent, and 5-15 parts of modified inorganic particles are added to a high-speed mixer and mixed evenly to obtain a mixture; the mixture is then added to a twin-screw extruder for co-melt extrusion to obtain the high-elasticity composite polymer material.

[0014] The modified polyurethane is prepared by polycondensation of diisocyanate and hydroxyl-terminated polydimethylsiloxane, chain extension of polyethylene glycol, and end-capping reaction with an end-capping agent; wherein the molar ratio of diisocyanate to hydroxyl-terminated polydimethylsiloxane is 1-1.6:1.

[0015] A mixed rubber is prepared by condensing hydroxyl-terminated polydimethylsiloxane silicone rubber and toughening rubber in a ratio of 1-2:1-2 with the diisocyanate; 2-6 parts of reinforcing agent and 2 parts of sulfur are added to the mixed rubber, and the mixture is then molded to obtain the modified rubber; wherein the ratio of the diisocyanate to the total parts of the hydroxyl-terminated polydimethylsiloxane silicone rubber and toughening rubber is 0.8-1.2:1.

[0016] The modified inorganic particles were prepared by adding a silane coupling agent to the inorganic particles;

[0017] The capping agent was prepared by reacting 2-(2-chlorophenyl)-4,6-diphenyl-1,3,5-triazine with 4-hydroxyphenylboronic acid.

[0018] The lubricant is selected from zinc stearate; the antioxidant is selected from antioxidant 1010.

[0019] Preferably, the preparation of the capping agent includes the following steps:

[0020] The 2-(2-chlorophenyl)-4,6-diphenyl-1,3,5-triazine, the 4-hydroxyphenylboronic acid, tetratriphenylphosphine palladium, and cesium carbonate were added to 1,4-dioxane and reacted at 100°C for 6 hours to obtain a reaction solution. The reaction solution was cooled, diluted with water and ethyl acetate, extracted and separated, distilled under reduced pressure, and dried to obtain the end-capping agent.

[0021] The amount of the capping agent used is 2-6 parts.

[0022] Preferably, the operating parameters of the twin-screw extruder are as follows: screw speed is 500 r / min, feed speed is 30 r / min, and the temperatures of the first to eighth temperature zones are 200℃, 205℃, 210℃, 215℃, 220℃, 215℃, and 210℃, respectively, with the die head temperature being 210℃.

[0023] Preferably, the preparation of the modified polyurethane includes the following steps:

[0024] The diisocyanate and the hydroxyl-terminated polydimethylsiloxane were dried in a vacuum drying oven at 80°C for 2 hours to obtain a dried raw material; the hydroxyl-terminated polydimethylsiloxane and the diisocyanate were added to a four-necked flask and dissolved in DMF to obtain a dissolved system; the dissolved system was protected with nitrogen, heated to 50°C, and 1% molar amount of dibutyltin dilaurate was added and reacted for 3 hours to obtain a reaction system; the polyethylene glycol was added to the reaction system, and the chain extension reaction was carried out at 50°C for 2 hours to obtain a polyurethane prepolymer;

[0025] The polyurethane prepolymer was cooled to 40°C, acetone was added to reduce viscosity, and the end-capping agent was added. The end-capping reaction was carried out at 60°C to obtain an intermediate. The intermediate was cooled to room temperature, and triethylamine was added to the neutralization reaction system at 200 r / min. The reaction was carried out for 30 min to obtain a neutralized system. Epoxy resin was added to the neutralized system, and the reaction was carried out at 50°C for 1 h at 200 r / min to obtain a cured system. The cured system was then vacuum dried at 80°C for 2 h to obtain the modified polyurethane.

[0026] Preferably, the diisocyanate is selected from toluene diisocyanate, terephthalic diisocyanate, lysine diisocyanate, and hexamethylene diisocyanate.

[0027] Preferably, the preparation of the modified rubber includes the following steps:

[0028] Weigh the hydroxyl-terminated polydimethylsiloxane silicone rubber, the toughened rubber, and the diisocyanate into a three-necked flask, dissolve them in chloroform, heat to 100°C and stir for 30 min, add dibutyltin dilaurate, and react for 2 h to obtain a mixed rubber.

[0029] The mixed rubber is plasticized in an open mill for 10 minutes, the reinforcing agent is added, the temperature is maintained at 70°C, and the mixture is mixed for 20 minutes to obtain a mixed rubber; sulfur is added to the mixed rubber, the temperature is raised to 110°C and the rubber is discharged, and the sheet is obtained to obtain a compound rubber; the compound rubber is cooled to room temperature and left for 24 hours, and then molded on a flat vulcanizing machine to obtain the modified rubber.

[0030] Preferably, the toughening rubber is selected from styrene-butadiene rubber, ethylene propylene rubber, nitrile rubber, and butadiene rubber.

[0031] Preferably, the toughening agent is selected from one of ethylene-vinyl acetate copolymer, acrylonitrile-butadiene-styrene copolymer, styrene-butadiene-styrene block copolymer, and chlorinated polyethylene.

[0032] Preferably, the preparation of the modified inorganic particles includes the following steps:

[0033] The inorganic particles were added to a three-necked flask and dissolved in a mixture of ethanol and water (V alcohol:V water = 5:1) to obtain a mixed solution. The mixed solution was adjusted to a weakly acidic state with glacial acetic acid, ultrasonically dispersed for 30 min, and the silane coupling agent was added. The mixture was stirred and reacted for 6 h in a water bath at 85 °C to obtain the modified inorganic particles.

[0034] Preferably, the inorganic particles are selected from one of graphene oxide, nano-titanium dioxide, nano-silicon carbide, and nano-silicon dioxide; the silane coupling agent is selected from one of 3-aminopropyltriethoxysilane, 3-(2,3-epoxypropoxy)propyltrimethoxysilane, methacryloyloxypropyltriethoxysilane, and N-(2-aminoethyl)-3-aminopropyltrimethoxysilane.

[0035] Another aspect of the present invention provides a highly elastic composite polymer material, comprising modified polyurethane, modified rubber, lubricant, antioxidant, toughening agent, and modified inorganic particles; the highly elastic composite polymer material is prepared by any one of the preparation methods described above; the tensile strength of the highly elastic composite polymer material is 85.2 MPa, the elongation at break is 68.5%; the elastic recovery rate at 30% constant elongation is 98.8%; the impact strength of the highly elastic composite polymer material is 95.2 MPa; the tensile strength retention rate of the highly elastic composite polymer material after irradiation at 80°C for 800 h is 98.6%; the tensile strength of the highly elastic composite polymer material at 200°C is 92.5 MPa.

[0036] Compared with the prior art, the beneficial effects of the present invention are as follows:

[0037] 1. This invention prepares modified polyurethane by condensing diisocyanate with polysiloxane, chain extension with polyethylene glycol, and end-capping reaction with an end-capping agent. Silicone rubber and toughening rubber are polymerized using diisocyanate. A reinforcing agent is added to the resulting mixed rubber, which is then vulcanized to obtain modified rubber. Finally, the modified polyurethane and modified rubber are melt-extruded to obtain an elastic composite polymer material. By controlling the type and amount of diisocyanate and the average molecular weight of polyethylene glycol, the resulting high-elasticity composite polymer material exhibits a tensile strength of 85.2 MPa and an elongation at break of 68.5%, demonstrating improved tensile strength.

[0038] 2. This invention utilizes reinforcing agents to significantly improve the elastic modulus of modified rubber, thereby enhancing its resistance to deformation. Simultaneously, modified polyurethane provides polyethylene glycol soft segments and the flexibility of Si-O bonds, further improving the material's elastic properties. By using carbon nanotubes as reinforcing agents and controlling the amounts of modified polyurethane and modified rubber, the resulting high-elasticity composite polymer material exhibits an elastic recovery rate of 98.8% at 30% constant elongation, demonstrating improved elastic properties.

[0039] 3. This invention modifies silicone rubber by adding toughening rubber. At the same time, the addition of toughening agent can induce the formation of crazes and shear bands. The generation and development of crazes and shear bands consume a lot of energy, thereby improving the strength of the composite material. By controlling the type and amount of toughening rubber and adjusting the type and amount of toughening agent, the impact strength of the obtained high-elasticity composite polymer material is 95.2 MPa, which is an improvement in impact strength.

[0040] 4. This invention uses 2-(2-chlorophenyl)-4,6-diphenyl-1,3,5-triazine as a capping agent to introduce triazine-based UV absorbers into the polyurethane backbone. The UV absorber's ability to capture free radicals increases the aging resistance of the composite material. Simultaneously, nano-titanium dioxide is introduced, utilizing its UV-shielding properties to synergistically improve the material's aging resistance. By changing the amount of capping agent and modified polyurethane, the resulting high-elasticity composite polymer material retains 98.6% of its tensile strength after 80°C irradiation for 800 hours, demonstrating improved anti-aging performance.

[0041] 5. This invention improves the strength and toughness of materials by adding modified inorganic particles during the melt extrusion process of modified rubber and modified polyurethane, utilizing the high specific surface area and high modulus of nano-inorganic particles. At the same time, the energy applied to the composite material under high temperature environment is dissipated due to the chemical bonding or physical adsorption between the nanoparticles and the material, thus improving the heat resistance of the material. The high-elasticity composite polymer material prepared using KH-792 modified nano-titanium dioxide has a tensile strength of 92.5 MPa at 200℃, and its heat resistance is improved. Attached Figure Description

[0042] Figure 1 shows the changes in elastic recovery rate under the condition of 10%-50% elongation in Examples 15 and 22-24.

[0043] Figure 2 shows the changes in tensile strength before and after aging treatment in Examples 43-47. Detailed Implementation

[0044] The technical solutions of the embodiments of the present invention will be clearly and completely described below with reference to the accompanying drawings. Obviously, the described embodiments are only some embodiments of the present invention, and not all embodiments. Based on the embodiments of the present invention, all other embodiments obtained by those skilled in the art without creative effort are within the scope of protection of the present invention.

[0045] Please refer to Figures 1 and 2. This invention provides a highly elastic composite polymer material and its preparation process, the technical solution of which is as follows:

[0046] The EVA described in this invention is an ethylene-vinyl acetate copolymer; the ABS is an acrylonitrile-butadiene-styrene copolymer; the SBS is a styrene-butadiene-styrene block copolymer; and the CPE is chlorinated polyethylene.

[0047] The present invention describes KH-550 as 3-aminopropyltriethoxysilane; KH-560 as 3-(2,3-epoxypropoxy)propyltrimethoxysilane; KH-570 as methacryloyloxypropyltriethoxysilane; and KH-792 as N-(2-aminoethyl)-3-aminopropyltrimethoxysilane.

[0048] Example 1

[0049] Add 5 mmol of 2-(2-chlorophenyl)-4,6-diphenyl-1,3,5-triazine, 6 mmol of 4-hydroxyphenylboronic acid, 0.02 mmol of tetraphenylphosphine palladium, and 10 mmol of cesium carbonate to 5 ml of 1,4-dioxane, and react at 100 °C for 6 h to obtain a reaction solution; cool the reaction solution, dilute with water and ethyl acetate, extract and separate, distill under reduced pressure, and dry to obtain the end-capping agent.

[0050] Toluene diisocyanate and hydroxyl-terminated polydimethylsiloxane were dried in a vacuum drying oven at 80°C for 2 hours to obtain a dried raw material. The dihydroxyl-terminated polydimethylsiloxane and the toluene diisocyanate were added to a four-necked flask and dissolved in 2 ml of DMF to obtain a solution system. The solution system was protected with nitrogen, heated to 50°C, and 1% dibutyltin dilaurate was added and reacted for 3 hours to obtain a reaction system. Polyethylene glycol with a molar ratio of 5:1 to diisocyanate was added to the reaction system, and the reaction was carried out at 50°C for 2 hours to obtain a chain extension reaction, thus obtaining a polyurethane prepolymer.

[0051] The polyurethane prepolymer was cooled to 40°C, acetone was added to reduce viscosity, and 5 parts of the capping agent were added. The capping reaction was carried out at 60°C to obtain an intermediate. The intermediate was cooled to room temperature, and triethylamine was added to the neutralization reaction system at 200 r / min. The reaction was carried out for 30 min to obtain a neutralized system. 5 parts of epoxy resin were added to the neutralized system, and the system was cured at 80°C at 200 r / min for 1 h to obtain a cured system. The cured system was vacuum dried at 80°C for 2 h to obtain modified polyurethane.

[0052] Weigh 50 parts of hydroxyl-terminated polydimethylsiloxane silicone rubber, 50 parts of styrene-butadiene rubber, and 50 parts of toluene diisocyanate and add them to a three-necked flask. Dissolve them in 5 ml of chloroform, heat to 100℃ and stir for 30 min. Add 5 parts of dibutyltin dilaurate and react for 2 h to obtain a mixed rubber.

[0053] 100 parts of the mixed rubber were plasticized on an open mill for 10 minutes, 5 parts of carbon nanotubes were added, and the temperature was maintained at 70℃ for 20 minutes to obtain a mixed rubber. 2 parts of sulfur were added to the mixed rubber, the temperature was raised to 110℃, and the rubber was discharged and sheeted to obtain a compound. The compound was cooled to room temperature and left for 24 hours. The positive vulcanization time t90 of the compound was tested using an MDR-2000E rotorless vulcanizing apparatus. Then, under conditions of 153℃ * t90 and 10MPa pressure, the compound was molded on an XLB-50T2 flat vulcanizing machine to obtain modified rubber.

[0054] 60 parts of the modified rubber, 90 parts of the modified polyurethane, 5 parts of zinc stearate, 5 parts of antioxidant 1010, and 15 parts of ethylene-vinyl acetate copolymer were added to a high-speed mixer and mixed evenly to obtain a mixture. The mixture was then added to a twin-screw extruder for blending and melt extrusion to obtain the high-elasticity composite polymer material.

[0055] Examples 2-12 follow the same preparation method and parameter conditions as Example 1, with differences shown in Table 1.

[0056] Table 1. Differences in parameters between Examples 1-12 and Comparative Examples 1-2

[0057] Example 2: Types of Isocyanates n（二异氰酸酯） The ratio of n-(hydroxyl-terminated polydimethylsiloxane) rubber to diisocyanate and the average molecular weight of polyethylene glycol are shown in the following examples: Example 1: Toluene diisocyanate 1.5:11:11600; Example 2: Terephthalic dimethyl diisocyanate 1.5:11:11600; Example 3: Lysine diisocyanate 1.5:11:11600; Example 4: Hexamethylene diisocyanate 1.5:11:11600; Example 5: Hexamethylene diisocyanate 1:11:11600; Example 6: Hexamethylene diisocyanate Example 7: Hexamethylene diisocyanate 1.6:11:11600; Example 8: Hexamethylene diisocyanate 1.5:10.8:11600; Example 9: Hexamethylene diisocyanate 1.5:11.2:11600; Example 10: Hexamethylene diisocyanate 1.5:11:1800; Example 11: Hexamethylene diisocyanate 1.5:11:11200; Example 12: Hexamethylene diisocyanate 1.5:11:11800

[0058] Comparative Example 1 follows the same preparation method and parameters as Example 1, except that it does not use mixed rubber, but only polydimethylsiloxane silicone rubber.

[0059] Comparative Example 2 follows the same preparation method and parameters as Example 1, except that it does not use a polyethylene glycol chain extension reaction.

[0060] Example 13 Tensile property test

[0061] The high-elasticity composite polymer materials prepared in Examples 1-12 and Comparative Examples 1-2 were subjected to tensile property tests using a universal testing machine (XWW-20A). The tensile strength and elongation at break of the materials were tested. The tests were conducted in accordance with GB / T228.1-2010. During the tests, the test specimens were stably fixed using clamping devices, and the tensile rate was set to 20 mm / min. The test results are shown in Table 2.

[0062] Table 2 Tensile strength tests of Examples 1-12 and Comparative Examples 1-2

[0063] Example 1: Tensile Strength / MPa, Elongation at Break / % Example 2: 72.4, 56.2 Example 3: 76.5, 65.8 Example 4: 85.2, 68.5 Example 5: 72.8, 52.7 Example 6: 80.3, 66.2 Example 7: 85.5, 67.6 Example 8: 84.6, 66.2 Example 9: 85.1, 67.8 Example 10: 88.2, 58.2 Example 11: 86.5, 63.8 Example 12: 72.8, 69.6 Comparative Example 1: 60.1, 28.6 Comparative Example 2: 55.4, 15.8

[0064] As shown in Table 2, the tensile strength and elongation at break of the polymer materials obtained by melt extrusion of the modified rubber and modified polyurethane prepared using a single rubber material in Comparative Example 1 were significantly lower than those in Examples 1-12. In Comparative Example 2, the modified polyurethane prepared without the addition of polyethylene glycol for chain extension resulted in a significant decrease in elongation at break and tensile strength of the polymer material obtained by melt extrusion. The addition of polyethylene glycol increased the content of the polyurethane soft segments, which can disperse external forces under external force, ensuring uniform stress distribution and preventing material fracture, thus improving tensile strength and elongation at break. The results of Examples 1-4 show that the composite material prepared using hexamethylene diisocyanate exhibits significantly improved tensile strength and elongation at break. Because long-chain isocyanates can effectively reduce the applied force, the stress can be dispersed in the aliphatic linear chain, increasing tensile strength. Simultaneously, the dispersed force can improve the material's ductility and elongation at break. Aromatic isocyanates, due to their cyclic rigid structure, can increase the tensile strength of the material, but due to the conjugation effect, the applied external force further strengthens the structure. The intermolecular forces in the system reduce the elongation at break. Lysine diisocyanate, due to its short chain, has limited dispersing forces, exhibiting lower tensile strength and elongation at break. Results from Examples 4-7 show that with increasing molar ratio of diisocyanate to dihydroxypolydimethylsiloxane, tensile strength gradually increases and tends to stabilize, while elongation at break shows a trend of first increasing and then decreasing. With decreasing content of dihydroxypolydimethylsiloxane, the flexibility effect of Si-O bonds in the material gradually weakens, leading to a decrease in elongation at break. Examples 4 and 7... The results of Examples 8-9 show that as the ratio of rubber to diisocyanate increases, the tensile strength and elongation at break change little and tend to stabilize. Since the rubber material is connected by diisocyanate in an equal proportion, a small increase in the ratio has little effect on the tensile properties. The results of Examples 4 and 10-12 show that as the average molecular weight of polyethylene glycol increases, the tensile strength of the material gradually decreases, and the elongation at break shows a trend of first increasing and then decreasing. Due to the increase in molecular weight, the force dispersion effect is weakened, and it is easy to break under external force. The results in Table 2 show that by controlling the type and amount of diisocyanate and the average molecular weight of polyethylene glycol, the tensile strength of the high-elasticity composite polymer material is 85.2 MPa and the elongation at break is 68.5%.

[0065] Example 14

[0066] 100 parts of the mixed rubber were plasticized on an open mill for 10 minutes, 5 parts of carbon nanotubes were added, and the temperature was maintained at 70℃ for 20 minutes to obtain a mixed rubber. 2 parts of sulfur were added to the mixed rubber, the temperature was raised to 110℃, and the rubber was discharged and sheeted to obtain a compound. The compound was cooled to room temperature and left for 24 hours. The positive vulcanization time t90 of the compound was tested using an MDR-2000E rotorless vulcanizing apparatus. Then, under conditions of 153℃ * t90 and 10MPa pressure, the compound was molded on an XLB-50T2 flat vulcanizing machine to obtain modified rubber.

[0067] The highly elastic composite polymer material was prepared according to Example 4.

[0068] Examples 15-27 follow the same preparation method and parameters as in Example 14, with differences shown in Table 3.

[0069] Comparative Example 3 follows the same preparation method and parameters as Example 14, except that no reinforcing agent is added.

[0070] Comparative Example 4 follows the same preparation method and parameters as Example 14, except that no modified polyurethane is added.

[0071] Example 28 Elasticity property determination

[0072] Tensile tests with a fixed elongation of 5%-30% were conducted using an INSTRON 5843 universal tensile testing machine manufactured in the United States, with a clamping distance of 100 mm and a tensile speed of 500 mm / min. The formula for calculating the elastic recovery rate is shown below.

[0073] Elastic recovery rate (%) = L0 - L2 / L0 × 100%

[0074] In the formula: L0 is the set elongation value of the material; L2 is the elongation value corresponding to the material being stretched again to the pre-tension after relaxation recovery. The elastic recovery rate when the fixed elongation is 30% is shown in Table 3; the elastic recovery rate variation graphs of Examples 15 and Examples 22-24 under the condition of fixed elongation of 10%-50% are shown in Figure 1.

[0075] Table 3 Elastic property determination of Examples 14-27 and Comparative Examples 3-4

[0076] Example 1: Modified polyurethane dosage (parts); Modified rubber dosage (parts); Reinforcing agent type; Reinforcing agent dosage (parts); Elastic recovery rate (%). Example 1: 46060 carbon nanotubes; 593.6%; Example 1: 159060 carbon nanotubes; 598.8%; Example 1: 167060 carbon nanotubes; 595.2%; Example 17: 178060 carbon nanotubes; 596.4%; Example 18: 10060 carbon nanotubes; 598.9%; Example 19: 199040 carbon nanotubes; 592.5%; Example 20: 9050 carbon nanotubes. Example 21: 594.5g carbon nanotube; Example 22: 596.5g carbon nanotube; Example 23: 597.2g graphene; Example 24: 596.9g silica; Example 25: 596.6g carbon fiber; Example 26: 292.6g carbon nanotube; Example 27: 699.1g carbon nanotube; Comparative Example 3: 39060 / / 75.6g carbon nanotube; Comparative Example 4: 580.2g carbon nanotube.

[0077] As shown in Figure 1, the elastic recovery rate of the composite material exhibits significant differences with changes in the type of reinforcing agent, under conditions of 10%-50% elongation. The elastic recovery rate gradually decreases with increasing elongation. Table 3 shows that the composite material obtained by melt extrusion of modified rubber without reinforcing agent in Comparative Example 3 has a significantly lower elastic recovery rate compared to the composite material obtained without modified polyurethane in Comparative Example 4. This is because the reinforcing agent can significantly increase the elastic modulus of the modified rubber, thereby improving its resistance to deformation. The modified polyurethane provides polyethylene glycol soft segments and the flexibility of Si-O bonds, further enhancing the material's elastic properties. The results of Examples 14-18 show that with increasing amounts of modified polyurethane, the elastic recovery rate of the composite material... The elastic recovery rate gradually increased and remained above 95%, further illustrating the characteristics of polyurethane soft segments and siloxane bonds in enhancing elastic properties. Examples 15 and 19-21 show that with the increase of modified rubber content, the elastic recovery rate of the composite material exhibits a trend of first increasing and then decreasing. Examples 15 and 22-24 show that with the change of reinforcing agent type, the elastic recovery rate of the composite material stabilized above 96%. The rod-like structure, large aspect ratio, and high elastic modulus of carbon nanotubes allow them to act as a skeleton in the material, increasing its hardness, improving load transfer and stress distribution, avoiding excessive local stress concentration, enhancing deformation resistance, and increasing the elastic recovery rate. Examples 15 and 25-27... The results show that as the amount of reinforcing agent increases, the elastic recovery rate gradually improves. However, excessive use of reinforcing agent causes aggregation between carbon nanotube molecules, further affecting the overall mechanical properties. As shown in Table 3 and Figure 1, the modified rubber prepared using carbon nanotubes as reinforcing agents has an elastic recovery rate of 98.8% at 30% constant elongation with the high-elasticity composite polymer material obtained by melt extrusion of modified polyurethane, demonstrating significantly improved elastic properties.

[0078] Example 29

[0079] Weigh 50 parts of hydroxyl-terminated polydimethylsiloxane silicone rubber, 50 parts of styrene-butadiene rubber, and 50 parts of toluene diisocyanate and add them to a three-necked flask. Dissolve them in 5 ml of chloroform, heat to 100℃ and stir for 30 min. Add 5 parts of the catalyst dibutyltin dilaurate and react for 2 h to obtain the mixed rubber.

[0080] The modified rubber was prepared according to Example 15.

[0081] 60 parts of the modified rubber, 90 parts of the modified polyurethane, 5 parts of zinc stearate, 5 parts of antioxidant 1010, and 15 parts of ethylene-vinyl acetate copolymer were added to a high-speed mixer and mixed evenly to obtain a mixture. The mixture was then added to a twin-screw extruder for blending and melt extrusion to obtain the high-elasticity composite polymer material.

[0082] Examples 30-40 follow the same preparation method and parameters as Example 29, with differences shown in Table 4.

[0083] Comparative Example 4 follows the same preparation method and parameters as Example 29, except that no toughening agent is added.

[0084] Comparative Example 5 follows the same preparation method and parameters as Example 29, except that toughening rubber is not added.

[0085] Example 41 Impact Performance Test

[0086] The highly elastic composite polymer materials prepared in Examples 29-40 and Comparative Examples 4-5 were subjected to impact strength testing using an impact testing machine (XJ-300A) according to the national standard GB / T1043.1-2008. Before impact, the prepared standard test specimens were stabilized and fixed with clamps. During impact, the pendulum of the impact testing machine was dropped at a 150° angle. The test results are shown in Table 4.

[0087] Table 4 Impact strength determination of Examples 29-40 and Comparative Examples 4-5

[0088] Examples | Toughening Rubber Type | Ratio of Toughening Rubber to Silicone Rubber | Toughening Agent Type | Toughening Agent Dosage / Parts | Impact Strength / MPa | Example 29 | Styrene-butadiene rubber 1:1 EVA 1595.2 | Example 30 | Ethylene-propylene rubber 1:1 EVA 1588.4 | Example 31 | Nitrile-butadiene rubber 1:1 EVA 1592.6 | Example 32 | Butadiene rubber 1:1 EVA 1585.8 | Example 33 | Styrene-butadiene rubber 1:2 EVA 1585.9 | Example 34 | Styrene-butadiene rubber 2:1 EVA 1 595.4 Example 35 Styrene-butadiene rubber 1:1 SBS 1591.5 Example 36 Styrene-butadiene rubber 1:1 ABS 1589.7 Example 37 Styrene-butadiene rubber 1:1 CPE 1592.6 Example 38 Styrene-butadiene rubber 1:1 EVA 584.3 Example 39 Styrene-butadiene rubber 1:1 EVA 1089.2 Example 40 Styrene-butadiene rubber 1:1 EVA 1892.5 Comparative Example 4 Styrene-butadiene rubber 1:1 / / 52.8 Comparative Example 5 / / EVA 1558.6

[0089] As shown in Table 2, the impact strength of the composite materials obtained in Comparative Examples 4 and 5 without toughening rubber and with toughening agent modification, respectively, only reached over 50%, exhibiting a significant decrease in impact resistance compared to Examples 29-40. The results of Examples 29-32 show that the impact strength of the composite materials made using styrene-butadiene rubber and nitrile rubber can reach over 90 MPa. The rigid structure of the benzene ring can further increase the impact resistance of the material. The addition of short-chain olefin rubber can enhance the tensile properties of the composite material, but it is not conducive to improving the impact performance. The results of Examples 29 and 33-34 show that the impact strength of the composite material gradually increases with the increase of toughening rubber content; however, the addition of excessive styrene-butadiene rubber will affect the tensile properties of the material. The results of Examples 29 and 35-37 show that the change in the type of toughening agent affects the impact strength of the material. Since the addition of toughening agent can induce the formation of crazes and shear bands, the generation and development of crazes and shear bands consume a large amount of energy, making the composite material... The strength of the material is improved, but the introduction of SBS and ABS increases the rigid groups in the composite material, reducing the overall mechanical properties of the material. Simultaneously, the excessive introduction of styrene and butadiene reduces the compatibility between the modified polyurethane and modified rubber in the composite material, thus reducing the impact performance. The results of Examples 29 and 38-40 show that with the increase of toughening agent dosage, the impact strength of the composite material exhibits a trend of first increasing and then decreasing. As the toughening agent dosage increases, the silver ripple branching and shear banding effects reach saturation, and the toughening effect gradually slows down. Excessive plasticizer reduces the compatibility between the composite material components, leading to a decrease in impact strength. The results in Table 4 show that using styrene-butadiene rubber as the toughening rubber and EVA as the toughening agent, with controlled dosage, the resulting high-elasticity composite polymer material has an impact strength of 95.2 MPa, exhibiting significantly improved impact resistance.

[0090] Example 42

[0091] Add 5 mmol of 2-(2-chlorophenyl)-4,6-diphenyl-1,3,5-triazine, 6 mmol of 4-hydroxyphenylboronic acid, 0.02 mmol of tetraphenylphosphine palladium, and 10 mmol of cesium carbonate to 1,4-dioxane, and react at 100 °C for 6 h to obtain a reaction solution; cool the reaction solution, dilute with water and ethyl acetate, extract and separate, distill under reduced pressure, and dry to obtain the end-capping agent.

[0092] Hexamethylene diisocyanate and dihydroxypolydimethylsiloxane were dried in a vacuum drying oven at 80°C for 2 hours to obtain a dried raw material. The dihydroxypolydimethylsiloxane and toluene diisocyanate were added to a four-necked flask and dissolved in 2 ml of DMF to obtain a dissolved system. Under nitrogen protection, the dissolved system was heated to 50°C and 1% dibutyltin dilaurate was added and reacted for 3 hours to obtain a reaction system. Polyethylene glycol was added to the reaction system and the reaction was carried out at 50°C for 2 hours to obtain a polyurethane prepolymer.

[0093] 50 parts of the polyurethane prepolymer were cooled to 40°C, acetone was added to reduce viscosity, and 5 parts of the end-capping agent were added. The end-capping reaction was carried out at 60°C to obtain an intermediate. The intermediate was cooled to room temperature, and triethylamine was added to the neutralization reaction system at 200 r / min. The reaction was carried out for 30 min to obtain a neutralization system. 5 parts of epoxy resin were added to the neutralization system, and the reaction was carried out at 80°C at 200 r / min for 1 h to obtain a cured system. The cured system was vacuum dried at 80°C for 2 h to obtain the modified polyurethane.

[0094] The highly elastic composite polymer material was prepared according to Example 29.

[0095] Examples 43-52 follow the same preparation method and parameters as Example 42, with differences shown in Table 5.

[0096] Comparative Example 6 follows the same preparation method and parameters as Example 42, except that no capping agent is added.

[0097] Example 53 Anti-aging performance test

[0098] The composite materials prepared in Examples 42-52 and Comparative Example 6 were placed in an ultraviolet aging test chamber for accelerated ultraviolet aging experiments. The test temperature was 80℃, the lamp source was an 800W high-pressure mercury lamp, the distance between the sample and the lamp source was 20mm, and the irradiation time was 800h. The tensile strength of the composite materials before and after irradiation was tested, and the strength retention rate was calculated. The changes in tensile strength before and after aging treatment in Examples 43-47 are shown in Figure 2, and the test results are shown in Table 5.

[0099] Table 5 Anti-aging performance tests of Examples 42-52 and Comparative Example 6

[0100] Example | Capping Agent Dosage / Parts | Modified Polyurethane Dosage / Parts | Curing Temperature / °C | Tensile Strength Retention Rate / % | Example 4 | 25708095.8 | Example 4 | 35908098.6 | Example 4 | 45608095.2 | Example 4 | 55808096.5 | Example 4 | 651008097.8 | Example 4 | 751208096.6 | Example 4 | 82908085.2 | Example 4 | 94908090.4 | Example 5 | 06908096.3 | Example 5 | 15907098.5 | Example 5 | 25909098.7 | Comparative Example 6 | 908065.2

[0101] As shown in Table 5, the composite material obtained by curing polyurethane prepolymer without adding the reaction product of 2-(2-chlorophenyl)-4,6-diphenyl-1,3,5-triazine as a capping agent in Comparative Example 6, and then melt-extruded with mixed rubber, showed significantly lower anti-aging performance compared to the composite material obtained in Examples 42-52. After irradiation at 80°C for 800 hours, the strength retention rate was only 65.2%. Figure 2 and the results of Examples 42-47 show that with the increase of modified polyurethane content, the strength retention rate of the composite material first increased and then decreased. Excessive modified polyurethane introduced a large number of polar groups, reducing the compatibility with the modified rubber and further reducing the anti-aging performance of the composite material. Examples 43 and 48- The results in Table 5 show that with the increase of the amount of end-capping agent, the strength retention rate of the composite material first increases and then decreases. The introduction of the end-capping agent increases the light stability of the composite material and reduces the influence of ultraviolet light on the intermolecular forces of the composite material. However, with the increase of end-capping agent, more non-polar groups are introduced into the composite material, which cannot form a stable cross-linked structure during the curing process. Under long-term ultraviolet light, the polar groups inside the material are oxidized by ultraviolet light, resulting in a decrease in tensile strength. The results of Examples 43 and 51-52 show that the change of curing temperature has little effect on anti-aging performance. However, excessively high temperature increases the degree of cross-linking and hydrogen bond density, further affecting the compatibility between modified polyurethane and modified rubber, and affecting the mechanical properties of the composite material. The results in Table 5 show that by changing the amount of end-capping agent and controlling the amount of modified polyurethane, the tensile strength retention rate of the prepared high-elasticity composite polymer material after irradiation at 80℃ for 800h is 98.6%, showing obvious anti-aging performance.

[0102] Example 54

[0103] 50 parts of graphene oxide were added to a three-necked flask and dispersed in 100 ml of a mixed solution of ethanol and water (V alcohol:V water = 5:1) to obtain a mixed solution; the mixed solution was adjusted to weak acidity with glacial acetic acid, ultrasonically dispersed for 30 min, 5 parts of KH-550 were added, and the mixture was stirred and reacted in a water bath at 85℃ for 6 h to obtain modified inorganic particles.

[0104] 60 parts of the modified rubber described in Example 43, 90 parts of the modified polyurethane, 12 parts of the modified inorganic particles, 5 parts of zinc stearate, 5 parts of antioxidant 1010, and 15 parts of EVA were added to a high-speed mixer and mixed evenly to obtain a mixture. The mixture was then added to a twin-screw extruder for blending and melt extrusion to obtain the high-elasticity composite polymer material.

[0105] Examples 55-63 follow the same preparation method and parameters as Example 54, with differences shown in Table 6.

[0106] Comparative Example 7 follows the same preparation method and parameters as Example 54, except that no modified inorganic particles are added.

[0107] Comparative Example 8 follows the same preparation method and parameters as Example 54, except that unmodified inorganic particles are added.

[0108] Example 64 Heat Resistance Test

[0109] The high-elasticity composite polymer materials prepared in Examples 54-63 and Comparative Examples 7-8 were subjected to tensile property testing using a universal testing machine with 5 mg samples, and the initial values ​​were recorded. The heating rate was controlled at 10℃ / min using a thermogravimetric analyzer, and the test temperature range was 0-200℃. After the materials cooled, the tensile properties were tested using a universal testing machine, and the tensile strength of the materials was tested. The test results are shown in Table 6.

[0110] Table 6 Heat resistance test results of Examples 54-63 and Comparative Examples 7-8

[0111] Examples | Silane Coupling Agent Type | Inorganic Particle Type | Modified Inorganic Particle Dosage / Parts | Tensile Strength Before Heating / MPa | Tensile Strength After Heating Treatment / MPa | Example 54KH-550 | Graphene Oxide | 129 | 1.2 | 8 | 1.4 | Example 55KH-560 | Graphene Oxide | 129 | 3.6 | 9 | 0.5 | Example 56KH-570 | Graphene Oxide | 129 | 1.8 | 8 | 2.9 | Example 57KH-792 | Graphene Oxide | 129 | 5.7 | 9 | 2.8 | Example 58KH-792 | Nano Titanium Dioxide | 129 | 5.492.5 Example 59 KH-792 nano titanium dioxide 1295.6 92.8 Example 60 KH-792 nano silicon carbide 1295.5 92.4 Example 61 KH-792 nano titanium dioxide 593.5 86.2 Example 62 KH-792 nano titanium dioxide 894.6 88.4 Example 63 KH-792 nano titanium dioxide 1595.8 92.3 Comparative Example 7 / / 85.2 65.8 Comparative Example 8 / nano titanium dioxide 1288.4 82.6

[0112] As shown in Table 6, the tensile strength of Comparative Example 7 (without modified inorganic particles) decreased significantly after heating compared to Comparative Example 8 (with unmodified inorganic particles), exhibiting poor heat resistance. Since modified inorganic particles crosslink polymer chains into a three-dimensional structure through chemical bonding or physical adsorption, the addition of high specific surface area and high modulus nanoparticles improves the strength and toughness of the material. Simultaneously, the energy applied to the material is dissipated due to the chemical bonding or physical adsorption between the nanoparticles and the material. At high temperatures, adsorption and desorption occur first between the composite material molecular chains and the nanoparticle surface, consuming energy and reducing the direct impact of temperature on the composite material molecules. Examples 54-63 showed a 95% retention rate of tensile strength before and after heating compared to Comparative Examples 7-8, demonstrating significantly improved heat resistance. The results of Examples 54-57 show that using other silane coupling agents resulted in poor hydrolysis performance of silane ethoxylates and graphene oxide. The weakening of the binding ability of olefins reduces the compatibility between molecules in the composite material, resulting in a significant decrease in heat resistance. The results of Examples 57-60 show that changes in inorganic particles have a relatively small impact on heat resistance, but the addition of nano-titanium dioxide can further improve the anti-aging properties of the composite material. The results of Examples 57 and 61-63 show that with the increase of the amount of modified inorganic particles, the tensile strength retention rate of the composite polymer material before and after heating gradually increases. When the amount of modified inorganic particles reaches 12 parts, the tensile strength retention rate reaches 96.9%. Further increasing the amount of modified inorganic particles results in a small change in the strength retention rate. However, the addition of excessive modified inorganic particles can cause the nanoparticles to agglomerate within the polymer material, further affecting the overall performance of the composite material. The results in Table 6 show that the high-elasticity composite polymer material prepared using KH-792 modified nano-titanium dioxide has a tensile strength of 92.5 MPa at 200℃, exhibiting significantly improved heat resistance.

[0113] Although embodiments of the invention have been shown and described, it will be understood by those skilled in the art that various changes, modifications, substitutions and alterations can be made to these embodiments without departing from the principles and spirit of the invention, the scope of which is defined by the appended claims and their equivalents.

Claims

1. A preparation process for a highly elastic composite polymer material, characterized in that: The preparation of the highly elastic composite polymer material includes the following steps: 60-120 parts of modified polyurethane, 40-70 parts of modified rubber, 5 parts of lubricant, 5 parts of antioxidant, 5-18 parts of toughening agent, and 5-15 parts of modified inorganic particles are added to a high-speed mixer and mixed evenly to obtain a mixture; the mixture is then added to a twin-screw extruder for co-melt extrusion to obtain the high-elasticity composite polymer material. The modified polyurethane is prepared by polycondensation of diisocyanate and hydroxyl-terminated polydimethylsiloxane, chain extension of polyethylene glycol, and end-capping reaction with an end-capping agent; wherein the molar ratio of diisocyanate to hydroxyl-terminated polydimethylsiloxane is 1-1.6:

1. Hydroxyl-terminated polydimethylsiloxane silicone rubber and toughening rubber are mixed in a ratio of 1-2:1-2, and then condensed with the diisocyanate to obtain a mixed rubber; 2-6 parts of reinforcing agent and 2 parts of sulfur are added to the mixed rubber, and the modified rubber is prepared by compression molding; wherein the ratio of diisocyanate to total rubber is 0.8-1.2:

1. The modified inorganic particles were prepared by adding a silane coupling agent to the inorganic particles; The capping agent was prepared by reacting 2-(2-chlorophenyl)-4,6-diphenyl-1,3,5-triazine with 4-hydroxyphenylboronic acid. The lubricant is selected from zinc stearate; the antioxidant is selected from antioxidant 1010.

2. The preparation process of a highly elastic composite polymer material according to claim 1, characterized in that: The preparation of the capping agent includes the following steps: The 2-(2-chlorophenyl)-4,6-diphenyl-1,3,5-triazine, the 4-hydroxyphenylboronic acid, tetratriphenylphosphine palladium, and cesium carbonate were added to 1,4-dioxane and reacted at 100°C for 6 hours to obtain a reaction solution. The reaction solution was cooled, diluted with water and ethyl acetate, extracted and separated, distilled under reduced pressure, and dried to obtain the end-capping agent. The amount of the capping agent used is 2-6 parts.

3. The preparation process of a highly elastic composite polymer material according to claim 1, characterized in that: The preparation of the modified polyurethane includes the following steps: The diisocyanate and the hydroxyl-terminated polydimethylsiloxane were dried in a vacuum drying oven at 80°C for 2 hours to obtain a dried raw material; the dried raw material was added to a four-necked flask and dissolved in DMF to obtain a dissolved system; the dissolved system was protected with nitrogen, heated to 50°C, and 1% molar amount of dibutyltin dilaurate was added and reacted for 3 hours to obtain a reaction system; the polyethylene glycol was added to the reaction system, and the chain extension reaction was carried out at 50°C for 2 hours to obtain a polyurethane prepolymer; The polyurethane prepolymer was cooled to 40°C, acetone was added to reduce viscosity, and the end-capping agent was added. The end-capping reaction was carried out at 60°C to obtain an intermediate. The intermediate was cooled to room temperature, and triethylamine was added to the neutralization reaction system at 200 r / min. The reaction was carried out for 30 min to obtain a neutralized system. Epoxy resin was added to the neutralized system, and the reaction was carried out at 50°C for 1 h at 200 r / min to obtain a cured system. The cured system was then vacuum dried at 80°C for 2 h to obtain the modified polyurethane.

4. The preparation process of a highly elastic composite polymer material according to claim 1, characterized in that: The diisocyanate is selected from one of toluene diisocyanate, terephthalic diisocyanate, lysine diisocyanate, and hexamethylene diisocyanate.

5. The preparation process of a highly elastic composite polymer material according to claim 1, characterized in that: The preparation of the modified rubber includes the following steps: The hydroxyl-terminated polydimethylsiloxane silicone rubber, the toughened rubber, and the diisocyanate were added to a three-necked flask, dissolved in chloroform, heated to 100°C and stirred for 30 min, then dibutyltin dilaurate was added and reacted for 2 h to obtain the mixed rubber. The mixed rubber is plasticized in an open mill for 10 minutes, the reinforcing agent is added, the temperature is maintained at 70°C, and the mixture is mixed for 20 minutes to obtain a mixed rubber; sulfur is added to the mixed rubber, the temperature is raised to 110°C and the rubber is discharged, and the sheet is obtained to obtain a compound rubber; the compound rubber is cooled to room temperature and left for 24 hours, and then molded on a flat vulcanizing machine to obtain the modified rubber.

6. The preparation process of a highly elastic composite polymer material according to claim 1, characterized in that: The toughening rubber is selected from one of styrene-butadiene rubber, ethylene propylene rubber, nitrile rubber, and butadiene rubber.

7. The preparation process of a highly elastic composite polymer material according to claim 1, characterized in that: The toughening agent is selected from one of ethylene-vinyl acetate copolymer, acrylonitrile-butadiene-styrene copolymer, styrene-butadiene-styrene block copolymer, and chlorinated polyethylene.

8. The preparation process of a highly elastic composite polymer material according to claim 1, characterized in that: The preparation of the modified inorganic particles includes the following steps: The inorganic particles were added to a three-necked flask, and a mixed solution of ethanol and water (V alcohol:V water = 5:1) was added to disperse the particles and obtain a mixed solution. The mixed solution was adjusted to weak acidity with glacial acetic acid, ultrasonically dispersed for 30 min, and the silane coupling agent was added. The mixture was stirred and reacted for 6 h in a water bath at 85 °C to obtain the modified inorganic particles.

9. The preparation process of a highly elastic composite polymer material according to claim 1, characterized in that: The inorganic particles are selected from one of graphene oxide, nano-titanium dioxide, nano-silicon carbide, and nano-silicon dioxide; the silane coupling agent is selected from one of 3-aminopropyltriethoxysilane, 3-(2,3-epoxypropoxy)propyltrimethoxysilane, methacryloyloxypropyltriethoxysilane, and N-(2-aminoethyl)-3-aminopropyltrimethoxysilane.

10. A highly elastic composite polymer material, characterized in that: The highly elastic composite polymer material comprises modified polyurethane, modified rubber, lubricant, antioxidant, toughening agent, and modified inorganic particles; the highly elastic composite polymer material is prepared by the preparation process described in any one of claims 1-9; the tensile strength of the highly elastic composite polymer material is 85.2 MPa, and the elongation at break is 68.5%; the elastic recovery rate of the highly elastic composite polymer material at 30% constant elongation is 98.8%; the impact strength of the highly elastic composite polymer material is 95.2 MPa; the tensile strength retention rate of the highly elastic composite polymer material after irradiation at 80°C for 800 h is 98.6%; the tensile strength of the highly elastic composite polymer material at 200°C is 92.5 MPa.

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