Improving recyclability and strengthening toughening thermosetting elastomers by mismatched supramolecular effects and their preparation and application

Abstract

The present invention proposes a thermosetting elastomer that utilizes mismatch supramolecular effects to improve recyclability and enhance toughening, and its preparation and application. The preparation method of the thermosetting elastomer of the present invention comprises the steps of: preparing a prepolymer; adding a mixed chain extender to carry out a chain extension reaction; and finally obtaining a thermosetting elastomer through a curing cross-linking reaction; the mixed chain extender is a combination of 4,4'-diaminodiphenylmethane (EDA) and isophthalic acid hydrazide (IPDH). The present invention introduces mismatch supramolecular interactions into the thermosetting elastomer to achieve enhancement and toughening, while significantly improving its multiple recyclability. The method of the present invention is simple, has low production cost, and has high practical applicability.

Description

Technical Field

[0001] The invention relates to the technical field of high-performance polymer material synthesis, and in particular to a thermosetting elastomer which utilizes mismatched supramolecular effects to improve recyclability and enhance toughness, and the preparation and application thereof. Background Art

[0002] The information disclosed in this background technology section is only intended to enhance the understanding of the overall background of the invention, and should not necessarily be regarded as an admission or any form of suggestion that the information constitutes the prior art already known to a person skilled in the art.

[0003] Thermosetting polymers are generally polymer materials with a three-dimensional network structure of permanent covalent cross-linking sites. These permanent covalent cross-linking structures give the materials excellent strength and outstanding chemical resistance, and are widely used in daily life, military and space fields. The global annual production of thermosetting polymers has exceeded 65 million tons. However, due to their high cross-linking density, these materials have limitations in tensile properties and recyclability. It is reported that the maximum toughness of thermosetting materials is still less than 400MJ m -3 , which is significantly lower than the reported values ​​for thermoplastic materials (500-1200 MJ m -3 ). In addition, thermoset materials that retain a permanent shape after curing are difficult to reprocess from a mechanical, technical and economic point of view, which is not conducive to sustainable development or circular economy. To address these issues, researchers have begun to introduce dynamic covalent or non-covalent bonds into polymer networks to achieve chemical recycling. However, as the mechanical properties of thermoset materials increase, they become more difficult to recycle.

[0004] Therefore, the development of thermosetting materials with high strength and toughness that can be recycled multiple times remains a challenging task. Undoubtedly, these innovations will have a profound impact on multiple industries, and are expected to reduce environmental pollution levels and promote sustainable development. Summary of the invention

[0005] In order to solve the problem that thermosetting elastomers are difficult to have high strength and high toughness and can be recycled multiple times, the present invention proposes a thermosetting elastomer that utilizes mismatch supramolecular interactions to improve recyclability and enhance toughness, and its preparation and application. The present invention introduces mismatch supramolecular interactions into thermosetting elastomers to achieve enhancement and toughening, while significantly improving its multiple recycling properties. The method of the present invention is simple, the production cost is low, and it has high practical applicability.

[0006] The present invention is achieved through the following technical solutions:

[0007] In a first aspect, the present invention provides a method for preparing a thermosetting elastomer that utilizes mismatched supramolecular effects to improve recyclability and enhance toughness, comprising the steps of: preparing a prepolymer; adding a mixed chain extender to carry out a chain extension reaction; and finally obtaining a thermosetting elastomer through a curing and cross-linking reaction; the mixed chain extender is a combination of 4,4'-diaminodiphenylmethane (EDA) and isophthalic acid hydrazide (IPDH).

[0008] According to the present invention, preferably, the thermosetting elastomer is a thermosetting poly(urethane-urea) elastomer.

[0009] Preferably, according to the present invention, the method for preparing the prepolymer comprises the steps of: in a solvent, under the action of a catalyst, reacting a diisocyanate and a diol to obtain a prepolymer.

[0010] Preferably, the solvent is one or a combination of two or more of N,N-dimethylformamide, N,N-dimethylacetamide, dimethyl sulfoxide, N-methylpyrrolidone or chloroform; the mass ratio of diisocyanate to solvent is 1:5-15.

[0011] Preferably, the catalyst is one or a combination of two or more of dibutyltin dilaurate (DBTDL), stannous octoate, bismuth isooctanoate, bismuth laurate, bismuth neodecanoate or bismuth cyclohexaneate; and the mass ratio of the catalyst to the diisocyanate is 0.04-0.1:1.

[0012] Preferably, the diisocyanate is selected from one or a combination of two or more of 4,4'-dicyclohexylmethane diisocyanate, isophorone diisocyanate, hexamethylene diisocyanate or diphenylmethane diisocyanate.

[0013] Preferably, the diol is selected from one or a combination of two or more of polytetrahydrofuran, polycaprolactone diol, polyethylene glycol or polypropylene glycol.

[0014] Preferably, the molar ratio of diisocyanate to diol is 1.5-3:1.

[0015] Preferably, the reaction temperature is 70-90° C., the reaction time is 2-4 h, and the reaction is carried out under stirring conditions.

[0016] Preferably according to the present invention, in the mixed chain extender, the molar ratio of 4,4'-diaminodiphenylmethane (EDA) to isophthalic acid hydrazide (IPDH) is 1:0.5-2.

[0017] Preferably according to the present invention, the molar ratio of the mixed chain extender to the diisocyanate used in the preparation of the prepolymer is 0.4-0.8:1.

[0018] Preferably, according to the present invention, the mixed chain extender is added to the reaction system in the form of a mixed chain extender solution; the solvent used in the mixed chain extender solution is one or a combination of two or more of N,N-dimethylformamide, N,N-dimethylacetamide, dimethyl sulfoxide, N-methylpyrrolidone or chloroform; the mass concentration of the mixed chain extender solution is 1-10%.

[0019] Preferably, according to the present invention, the chain extension reaction temperature is room temperature, the chain extension reaction time is 3-8 hours, and the chain extension reaction is carried out under stirring conditions.

[0020] Preferably, according to the present invention, before the curing reaction, a step of diluting the reaction solution with a diluent may be included. The diluent is one or a combination of two or more of N,N-dimethylformamide, N,N-dimethylacetamide, dimethyl sulfoxide, N-methylpyrrolidone or chloroform; the mass ratio of the diluent to the reaction solution is 1-2:1.

[0021] Preferably, according to the present invention, the curing cross-linking reaction comprises the steps of: adding a cross-linking agent solution dropwise to the reaction solution obtained by the chain extension reaction, mixing thoroughly, degassing, and then drying the solvent to obtain a thermosetting elastomer.

[0022] Preferably, the crosslinking agent is one or a combination of two or more of HT-100, trimethylolpropane, trimethylolpropane tris(3-mercaptopropionate) or pentaerythritol tetrakis-3-mercaptopropionate; the mass ratio of the crosslinking agent to the mass ratio of the diisocyanate used in the preparation of the prepolymer is 0.1-0.6:1, preferably 0.24-0.58:1, and more preferably 0.24:1.

[0023] Preferably, the solvent used for the crosslinker solution is one or a combination of two or more of N,N-dimethylformamide, N,N-dimethylacetamide, dimethyl sulfoxide, N-methylpyrrolidone or chloroform, and the mass concentration of the crosslinker solution is 5-10%.

[0024] Preferably, the conditions for drying the solvent are: drying at 70-90° C. for 10-15 h, and then drying at 90-110° C. for 6-10 h.

[0025] In a second aspect, the present invention provides a thermosetting elastomer obtained by the above preparation method, which utilizes mismatch supramolecular effects to improve recyclability and enhance toughness.

[0026] The third aspect of the present invention provides the use of the above-mentioned thermosetting elastomer in artificial tendons, shield machine sealing rings, corrosion-resistant transparent partitions, aircraft carrier deck anti-collision pads, and shock-absorbing pads.

[0027] The technical features and beneficial effects of the present invention are as follows:

[0028] (1) The thermosetting elastomer of the present invention uses a specific type of mixed chain extender in the preparation process, which achieves the enhancement and toughening of the thermosetting elastomer and the multiple recycling of the thermosetting elastomer. In addition, the thermosetting elastomer prepared by the method of the present invention has excellent tolerance to chemical media (such as organic solvents, etc.), creep and damage (such as puncture, fracture and impact).

[0029] (2) The supramolecular mixed chain extender with different stiffness used in the present invention can form a mismatched supramolecular effect (i.e., a mismatched combination of supramolecular effects). When the material is subjected to an external force, it can dissipate energy in a timely manner, thereby effectively avoiding excessive entanglement or excessive aggregation caused by the matching supramolecular effect, thereby toughening and strengthening the material while improving the recyclability of the material.

[0030] (3) The type of chain extender of the present invention is specific, and only the chain extender of the specific type and ratio of the present invention can achieve the excellent effect of the present invention; if the chain extender of the present invention is replaced, or one of the chain extenders of the present invention is replaced with some flexible chain extenders containing dynamic covalent bonds or other types of rigid chain extenders (such as 4,4'-diaminodiphenyl ketone), the mechanical properties and recycling performance of the resulting elastomer will be greatly reduced; if the ratio of the two chain extenders is not appropriate, the mechanical properties and recycling performance of the resulting elastomer will also be greatly reduced. The amount of the cross-linking agent used in the present invention also needs to be appropriate. Too much or too little will reduce the performance of the resulting material.

[0031] (4) The preparation method of the thermosetting elastomer of the present invention is simple and easy, the raw materials are easily available, the cost is low, and the requirements for the reaction conditions and the equipment used are not high.

[0032] (5) The strategy of enhancing toughness and improving multiple recycling performance through mismatched supramolecular effects provided by the present invention is not limited to thermosetting poly(urethane-urea) systems, but also has potential application value in enhancing toughness and improving multiple recycling performance of other thermosetting polymer materials. BRIEF DESCRIPTION OF THE DRAWINGS

[0033] Figure 1 It is a comparison chart of the mechanical properties of the elastomers prepared in Examples 1-3 and Comparative Examples 1-2.

[0034] Figure 2 It is a comparison chart of the recycling efficiency of the elastomers prepared in Example 1 and Comparative Examples 1-2 in three dimensions of toughness, stress and strain.

[0035] Figure 3 It is a comparison chart of the recycling efficiency of the elastomers prepared in Examples 1-3 in three dimensions: toughness, stress, and strain.

[0036] Figure 43 is a comparative diagram of the solvent resistance of the thermosetting elastomer prepared in Example 1 and the thermoplastic elastomer prepared in Comparative Example 3.

[0037] Figure 5 It is a comparison chart of the mechanical properties of the thermosetting elastomer prepared in Examples 4-5 and the thermoplastic elastomer (SPUU-IE) prepared in Comparative Example 3.

[0038] Figure 6 This is a comparison chart of the mechanical properties of the elastomers prepared in Comparative Examples 4-5. DETAILED DESCRIPTION

[0039] The present invention will be further described below in conjunction with specific examples. It should be understood that these examples are only used to illustrate the present invention and are not intended to limit the scope of the present invention. The experimental methods in the following examples without specifying specific conditions are usually carried out under conventional conditions or under conditions recommended by the manufacturer.

[0040] It should be noted that the terms used herein are only for describing specific embodiments and are not intended to limit the exemplary embodiments according to the present disclosure.

[0041] Terminology explanation:

[0042] PTMEG 2000: polytetrahydrofuran (number average molecular weight 2000), purchased from Aladdin Biochemical Technology Co., Ltd.;

[0043] HMDI: 4,4'-dicyclohexylmethane diisocyanate;

[0044] DBTDL: dibutyltin dilaurate, used as catalyst;

[0045] DMF: N,N-dimethylformamide;

[0046] THF: tetrahydrofuran;

[0047] AC: acetone;

[0048] DCM: dichloromethane;

[0049] EtOH: absolute ethanol;

[0050] EA: ethyl acetate;

[0051] n-Hex: n-hexane;

[0052] water: deionized water;

[0053] EDA: 4,4'-diaminodiphenylmethane;

[0054] IPDH: isophthaloyl dihydrazide;

[0055] HDES: bis(2-hydroxyethyl) disulfide;

[0056] BDO: 1,4-butanediol;

[0057] HT-100: aliphatic polyisocyanate trimer, purchased from Yantai Wanhua Chemical Group Co., Ltd.

[0058] Room temperature: has a meaning known in the art, generally refers to 25±2°C;

[0059] Mechanical properties test method: INSTRON 3344 electronic universal testing machine, cut the sample into a rectangular shape with a size of 25mm x 5mm x 0.6mm, and test at room temperature with a tensile rate of 50mm / min. Each sample is measured at least five times and the average value is taken;

[0060] Fracture strength: the ratio of the tensile force to the fracture cross-sectional area when the material breaks, i.e. stress;

[0061] Elongation at break: When a material is stretched to break by an external force, the ratio of the elongation after stretching to the length before stretching is called elongation at break, expressed as a percentage;

[0062] Toughness: refers to the ability of a material to absorb energy during plastic deformation and rupture.

[0063] Embodiment 1:

[0064] A method for preparing a thermosetting poly(urethane-urea) elastomer that improves recyclability and enhances toughness by utilizing mismatched supramolecular effects, comprising the steps of:

[0065] Add 2.62g HMDI (0.01mol), 10g PTMEG2000 (0.005mol), 150μL DBTDL (0.16g) and 22g anhydrous DMF to a 250mL round-bottom flask, heat in an 80℃ oil bath for 3h under magnetic stirring, turn off the heating, and wait for the system to cool to room temperature to obtain a prepolymer. Dissolve 0.003mol IPDH and 0.003mol EDA in 70g anhydrous DMF. Add a mixed DMF solution of IPDH and EDA to the prepolymer and react at room temperature for 5h under magnetic stirring. Then add 100g DMF for dilution and stir vigorously for 20min. Dissolve 0.62g HT-100 (crosslinker) in 10g DMF, add dropwise to the system, stir vigorously for 20min, and pour into a silicone mold for degassing. After the mold is removed until no more bubbles are generated, it is placed in an oven at 80°C for 12 hours for drying, and then placed in a vacuum oven at 100°C for 8 hours to further remove the residual DMF. The target thermosetting poly(urethane-urea) elastomer is obtained by demolding, which is denoted as SPUUN-IE.

[0066] Embodiment 2:

[0067] A method for preparing a thermosetting poly(urethane-urea) elastomer that improves recyclability and enhances toughness by utilizing mismatched supramolecular effects is as described in Example 1, except that the amount of IPDH used is 0.004 mol, the amount of EDA used is 0.002 mol; the other steps and conditions are the same as in Example 1. The obtained thermosetting poly(urethane-urea) elastomer is recorded as SPUUN-I2E.

[0068] Embodiment 3:

[0069] A method for preparing a thermosetting poly(urethane-urea) elastomer that improves recyclability and enhances toughness by utilizing mismatched supramolecular effects is as described in Example 1, except that the amount of IPDH used is 0.002 mol, the amount of EDA used is 0.004 mol; the other steps and conditions are the same as in Example 1. The obtained thermosetting poly(urethane-urea) elastomer is recorded as SPUUN-IE2.

[0070] Comparative Example 1:

[0071] A method for preparing a thermosetting poly(urethane-urea) elastomer is as described in Example 1, except that the amount of IPDH used is 0.006 mol, and EDA is not added; the other steps and conditions are the same as in Example 1. The obtained thermosetting poly(urethane-urea) elastomer is designated as SPUUN-I.

[0072] Comparative Example 2:

[0073] A method for preparing a thermosetting poly(urethane-urea) elastomer is as described in Example 1, except that the amount of EDA used is 0.006 mol, and IPDH is not added; the other steps and conditions are the same as in Example 1. The obtained thermosetting poly(urethane-urea) elastomer is denoted as SPUUN-E.

[0074] Embodiment 4:

[0075] A method for preparing a thermosetting poly(urethane-urea) elastomer that improves recyclability and strengthens toughness by using mismatched supramolecular effects is as described in Example 1, except that the amount of HT-100 used is 1.03 g; the other steps and conditions are the same as in Example 1. The obtained thermosetting poly(urethane-urea) elastomer.

[0076] Embodiment 5:

[0077] A method for preparing a thermosetting poly(urethane-urea) elastomer that improves recyclability and strengthens toughness by using mismatched supramolecular effects is as described in Example 1, except that the amount of HT-100 used is 1.53 g; the other steps and conditions are the same as in Example 1. The obtained thermosetting poly(urethane-urea) elastomer.

[0078] Comparative Example 3:

[0079] A method for preparing a thermoplastic poly(urethane-urea) is as described in Example 1, except that the DMF solution of HT-100 is not added; the other steps and conditions are the same as in Example 1. The obtained thermoplastic poly(urethane-urea) is denoted as SPUU-IE.

[0080] Comparative Example 4:

[0081] A method for preparing a thermosetting poly(urethane-urea) elastomer comprises the steps of:

[0082] Add 2.62g HMDI (0.01mol), 10g PTMEG2000 (0.005mol), 150μL DBTDL (0.16g) and 22g anhydrous DMF to a 250mL round-bottom flask, heat in an 80℃ oil bath for 3h under magnetic stirring, turn off the heating, and wait for the system to cool to room temperature to obtain a prepolymer. Dissolve 0.003mol IPDH and 0.003mol HDES in 70g anhydrous DMF. Add a mixed DMF solution of IPDH and HDES to the prepolymer and react at room temperature for 5h under magnetic stirring. Then add 100g DMF for dilution and stir vigorously for 20min. Dissolve 0.62g HT-100 (crosslinker) in 10g DMF, add dropwise to the system, stir vigorously for 20min, and pour into a silicone mold for degassing. After the mold is removed until no more bubbles are generated, it is placed in an 80°C oven for 12 hours for drying, and then placed in a 100°C vacuum oven for 8 hours to further remove the residual DMF. The target thermosetting poly(urethane-urea) elastomer is obtained by demolding. It is denoted as SPUUN IPDH-HDES .

[0083] Comparative Example 5:

[0084] A method for preparing a thermosetting poly(urethane-urea) elastomer comprises the steps of:

[0085] Add 2.62g HMDI (0.01mol), 10g PTMEG2000 (0.005mol), 150μL DBTDL (0.16g) and 22g anhydrous DMF to a 250mL round-bottom flask, heat in an 80℃ oil bath for 3h under magnetic stirring, turn off the heating, and wait for the system to cool to room temperature to obtain a prepolymer. Dissolve 0.003mol IPDH and 0.003mol BDO in 70g anhydrous DMF. Add a mixed DMF solution of IPDH and BDO to the prepolymer and react at room temperature for 5h under magnetic stirring. Then add 100g DMF for dilution and stir vigorously for 20min. Dissolve 0.62g HT-100 (crosslinker) in 10g DMF, add dropwise to the system, stir vigorously for 20min, and pour into a silicone mold for degassing. After the mold is removed until no more bubbles are generated, it is placed in an 80°C oven for 12 hours for drying, and then placed in a 100°C vacuum oven for 8 hours to further remove the residual DMF. The target thermosetting poly(urethane-urea) elastomer is obtained by demolding. It is denoted as SPUUN IPDH-BDO .

[0086] Test example

[0087] Figure 1 It is a comparison of the mechanical properties of the elastomers prepared in Examples 1-3 and Comparative Examples 1-2. As can be seen from the figure, when the mixed chain extender ratio is 1:1, the mismatch supramolecular content is the highest, the mismatch supramolecular effect is the strongest, and the mechanical properties are the best.

[0088] Figure 2 It is a comparison of the recycling efficiency of the elastomers prepared in Example 1 and Comparative Examples 1-2 in three dimensions of toughness, stress and strain. The recycling efficiency test method is as follows: test the toughness, stress and strain data of the original elastomer. Then cut the elastomer into pieces, put the elastomer fragments close together, and hot press for 1 hour under the conditions of 110°C and 20MPa to achieve recovery; continue to repeat the above steps three times; test the toughness, stress and strain of the recycled elastomer. The percentage of the toughness, stress and strain of the recycled elastomer to the toughness, stress and strain of the original elastomer is the recycling efficiency.

[0089] According to the bar graph, the efficiency of the thermosetting elastomer with mismatch supramolecular effect (SPUUN-IE) in three dimensions is much higher than that of the thermosetting elastomer without mismatch supramolecular effect (SPUUN-I, SPUUN-E).

[0090] Figure 3 The comparison of the recycling efficiency of the elastomers prepared in Examples 1-3 in three dimensions of toughness, stress and strain. The recycling efficiency test method is the same as above. According to the bar chart, the thermosetting elastomer (SPUUN-IE) with the highest content of mismatched supramolecular has the highest recycling efficiency in all three dimensions.

[0091] Figure 4 This is a comparison of the solvent resistance of the thermosetting elastomer (SPUUN-IE) prepared in Example 1 and the thermoplastic elastomer (SPUU-IE) prepared in Comparative Example 3. Specific test method: Cut the elastomer into small rectangular pieces (the mass of which is recorded as m1) and immerse them in different organic solvents. Keep them at room temperature for 48 hours without interference. Then take out the elastomer and wash it five times with excess solvent. Then place the elastomer in an oven at 120°C and dry it for 4 hours, weigh it and record it as m2. Calculate the gel fraction: gel fraction = m2 / m1×100%. By Figure 4 Analysis shows that the thermosetting SPUUN-IE is significantly more resistant to organic solvents than the thermoplastic SPUU-IE.

[0092] Figure 5 It is a comparison chart of the mechanical properties of the thermosetting elastomer prepared in Examples 4-5 and the thermoplastic elastomer (SPUU-IE) prepared in Comparative Example 3. As can be seen from the figure, the amount of crosslinking agent has a certain influence on the properties of the obtained material, and the mechanical properties of the thermoplastic elastomer (SPUU-IE) are the worst.

[0093] Figure 6 This is a comparison of the mechanical properties of the elastomers prepared in Comparative Examples 4-5. As can be seen from the figure, the mechanical properties of the elastomer prepared by mixing IPDH with flexible HDES or BDO are not as good as those of the elastomer mixed with IPDH and EDA.

Claims

1. A method for preparing a thermosetting elastomer that improves recyclability and enhances toughness by using mismatched supramolecular effects, comprising the steps of: preparing a prepolymer; adding a mixed chain extender to perform a chain extension reaction; and finally performing a curing and cross-linking reaction to obtain a thermosetting elastomer; The preparation method of the prepolymer comprises the following steps: in a solvent, under the action of a catalyst, diisocyanate and diol are reacted to obtain a prepolymer; the molar ratio of diisocyanate to diol is 1.5-3:1; The mixed chain extender is a combination of 4,4'-diaminodiphenylmethane (EDA) and isophthalic acid hydrazide (IPDH); the molar ratio of the mixed chain extender to the diisocyanate used in the preparation of the prepolymer is 0.4-0.8:1; The thermosetting elastomer is a thermosetting poly(urethane-urea) elastomer; in the mixed chain extender, the molar ratio of 4,4'-diaminodiphenylmethane (EDA) to isophthalic acid hydrazide (IPDH) is 1:0.5-2; the mass ratio of the crosslinking agent used for curing crosslinking to the mass ratio of the diisocyanate used in the preparation of the prepolymer is 0.1-0.6:

1.

2. The method for preparing a thermosetting elastomer by utilizing mismatched supramolecular effects to improve recyclability and enhance toughness according to claim 1, characterized in that: Includes one or more of the following conditions: i. Solvent N,N -dimethylformamide, N,N -Dimethylacetamide, dimethyl sulfoxide, N -Methyl pyrrolidone or chloroform, or a combination of two or more thereof; the mass ratio of diisocyanate to solvent is 1:5-15; ii. The catalyst is one or a combination of two or more of dibutyltin dilaurate (DBTDL), stannous octoate, bismuth isooctanoate, bismuth laurate, bismuth neodecanoate or bismuth cyclohexaneate; the mass ratio of the catalyst to the diisocyanate is 0.04-0.1:1; iii. diisocyanate is selected from one or a combination of two or more of 4,4'-dicyclohexylmethane diisocyanate, isophorone diisocyanate, hexamethylene diisocyanate or diphenylmethane diisocyanate; iv. a diol selected from one or a combination of two or more of polytetrahydrofuran, polycaprolactone diol, polyethylene glycol or polypropylene glycol; v. The reaction temperature is 70-90°C, the reaction time is 2-4h, and the reaction is carried out under stirring conditions.

3. The method for preparing a thermosetting elastomer by utilizing mismatched supramolecular effects to improve recyclability and enhance toughness according to claim 1, characterized in that: Includes one or more of the following conditions: i. The mixed chain extender is added to the reaction system in the form of a mixed chain extender solution; the solvent used for the mixed chain extender solution is N,N -dimethylformamide, N,N -Dimethylacetamide, dimethyl sulfoxide, N -Methyl pyrrolidone or chloroform, one or a combination of two or more; the mass concentration of the mixed chain extender solution is 1-10%; ii. The chain extension reaction temperature is room temperature, the chain extension reaction time is 3-8h, and the chain extension reaction is carried out under stirring conditions; iii. Before the curing reaction, the step of diluting the reaction solution with a diluent is included; the diluent is N,N -dimethylformamide, N,N -Dimethylacetamide, dimethyl sulfoxide, N -methyl pyrrolidone or chloroform, or a combination of two or more thereof; the mass ratio of the diluent to the reaction solution is 1-2:

1.

4. The method for preparing a thermosetting elastomer by utilizing mismatched supramolecular effects to improve recyclability and enhance toughness according to claim 1, characterized in that: The curing cross-linking reaction comprises the steps of: adding a cross-linking agent solution dropwise to the reaction solution obtained by the chain extension reaction, fully mixing, degassing, and then drying the solvent to obtain a thermosetting elastomer.

5. The method for preparing a thermosetting elastomer by utilizing mismatched supramolecular effects to improve recyclability and enhance toughness according to claim 4, characterized in that: Includes one or more of the following conditions: i. The crosslinking agent is one or a combination of two or more selected from HT-100, trimethylolpropane, trimethylolpropane tris(3-mercaptopropionate) or pentaerythritol tetrakis-3-mercaptopropionate; the mass ratio of the crosslinking agent to the mass ratio of the diisocyanate used in the preparation of the prepolymer is 0.24-0.58:1; ii. The solvent used for the crosslinking agent solution is N,N -dimethylformamide, N,N -Dimethylacetamide, dimethyl sulfoxide, N -Methylpyrrolidone or chloroform, one or a combination of two or more, the mass concentration of the crosslinker solution is 5-10%; iii. The conditions for drying the solvent are: drying at 70-90°C for 10-15 h, and then drying at 90-110°C for 6-10 h.

6. A thermosetting elastomer prepared by any one of claims 1 to 5, which utilizes mismatched supramolecular effects to improve recyclability and enhance toughness.

7. Application of the thermosetting elastomer prepared by any one of claims 1 to 5, which utilizes mismatched supramolecular effects to improve recyclability and enhance toughness, in artificial tendons, shield machine sealing rings, corrosion-resistant transparent partitions, aircraft carrier deck anti-collision pads, and shock-absorbing pads.

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