High tensile, room temperature self-healing and recyclable polyimine elastomers and methods of making the same

CN116554424BActive Publication Date: 2026-08-07SOUTH CHINA UNIV OF TECH
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Patent Information

Authority / Receiving Office
CN · China
Patent Type
Patents(China)
Current Assignee / Owner
SOUTH CHINA UNIV OF TECH
Filing Date
2023-05-04
Publication Date
2026-08-07

AI Technical Summary

Technical Problem

[0005]本发明的目的在于克服目前聚亚胺弹性体耐用性差、力学性能尤其是断裂伸长率较低以及废弃后无法有效处理而污染环境的缺点,提供了一种集高拉伸、室温自愈合和可回收性能于一体的聚亚胺弹性体的制备方法

Benefits of technology

[0017] (1) The high tensile, room temperature self-healing and recyclable polyimide elastomer obtained by the present invention has a tensile stress of 0.85-4.56 MPa and an elongation at break of 153-1110%, and a glass transition temperature of -72.6℃ to -45.3℃.

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Abstract

The application discloses a high-tensile, room-temperature self-healing and recyclable polyimine elastomer and a preparation method thereof. The preparation method takes a monomer A containing two amino groups, a small-molecule monomer B containing two aldehyde groups and adipic acid dihydrazide as raw materials, obtains a linear macromolecular prepolymer containing an imine bond through condensation reaction of the amino groups and the aldehyde groups, and then adds a crosslinking agent C to crosslink, so as to obtain the polyimine elastomer with high tensile, room-temperature self-healing and recyclable properties. The polyimine elastomer prepared by the application has the characteristics of green environmental protection and long service life, and has a good application prospect in the field of recyclable flexible electronic devices.
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Description

Technical Field

[0001] This invention belongs to the field of polymer material preparation technology, and in particular relates to a high-tensile, room-temperature self-healing and recyclable polyimide elastomer and its preparation method. Background Technology

[0002] In recent years, with increasing attention to sustainable development, the research and development of sustainable materials has become increasingly important. Polymer materials with self-healing and recyclable properties are a field of great interest. Traditional polymer materials, after being damaged, typically require manual repair or replacement, while self-healing polymer materials can automatically repair damage and restore their original properties, extending their service life. Furthermore, traditional thermosetting elastomer materials are often difficult to recycle, easily leading to resource waste and environmental pollution. Therefore, the development of self-healing and recyclable elastomer materials is of great significance.

[0003] Imine bonds are chemical bonds capable of dynamic recombination and are widely used in the design of self-healing polymer materials. Notably, imine bonds can hydrolyze in acidic environments to generate amino and aldehyde groups. Upon returning to a neutral or alkaline environment, the amino and aldehyde groups can recombine to form imine bonds, thus achieving recyclability. Chinese invention patent CN113583442A prepared a self-healing polyimide composite material with photothermal properties using dialdehyde, diamine, and triethylenetetramine in a specific ratio. This material exhibits a tensile stress as high as 40 MPa, but its elongation at break is low, only 6.5%. Moreover, this elastomer lacks recyclability and still faces the problem of non-degradability after disposal. Degradable polymer materials can decompose into smaller molecules under specific conditions, avoiding long-term environmental pollution. This helps mitigate the negative impacts of human activities on the environment and protect the stability of ecosystems and biodiversity. Currently, researchers have prepared polyimide materials with self-healing, degradable, and recyclable properties. For example, Zhao et al. prepared a thermosetting epoxy material based on epoxy groups and imine bonds using 3-methoxy-4-hydroxybenzaldehyde, p-aminophenol and epichlorohydrin. The material had a tensile stress of 42 MPa and an elongation at break of 4.1%. It was completely degraded after being immersed in a solution of N,N-dimethylformamide in concentrated hydrochloric acid at 65 °C for 30 min. After drying at 120 °C for 24 h, the recovered epoxy material was obtained, which had a tensile stress of 36 MPa and an elongation at break of 3.8% (ZHAO S, ABU-OMAR M M. Recyclable and Malleable Epoxy Thermoset Bearing Aromatic Imine Bonds[J]. Macromolecules,2018,51(23):9816-24). However, due to the lack of flexible molecular chain segments in its structure, this polyimide material has a high glass transition temperature (20-60℃), a low elongation at break (<100%), and a low healing efficiency at room temperature for 24 hours (43.7%). Its tensile properties and self-healing properties need to be improved, which greatly limits the application of polyimide materials.

[0004] Therefore, the preparation of an elastomer material based on imine bonds with high tensile strength, room temperature self-healing properties, and recyclability has become one of the hot topics and challenges in current materials science research. Summary of the Invention

[0005] The purpose of this invention is to overcome the shortcomings of current polyimide elastomers, such as poor durability, low mechanical properties (especially elongation at break), and environmental pollution due to ineffective disposal after disposal. This invention provides a method for preparing a polyimide elastomer that integrates high tensile strength, room temperature self-healing properties, and recyclability. The invention uses a monomer A containing two amino groups, a small molecule monomer B containing two aldehyde groups, and adipic acid dihydrazide to undergo a condensation reaction to obtain a prepolymer with a soft-hard segment structure based on dynamic imine bonds. This prepolymer is then reacted with a crosslinking agent C containing three aldehyde groups to obtain a polyimide elastomer with a low glass transition temperature, high elongation at break, and self-healing and recyclable properties.

[0006] The objective of this invention is achieved through the following technical solution:

[0007] A method for preparing a high-tensile, room-temperature self-healing, and recyclable polyimide elastomer specifically includes the following preparation steps:

[0008] Monomer A containing two amino groups, small molecule monomer B containing two aldehyde groups, and adipic acid dihydrazide are reacted at 25-80℃ for 2-6 hours to generate a linear macromolecular prepolymer containing dynamic imine bonds and hydrazide bonds. Then, a crosslinking agent C solution containing three aldehyde groups (crosslinking agent C is dissolved in an organic solvent) is added, and the reaction is continued at 25-80℃ for 12-24 hours. Finally, the reactants are poured into a polytetrafluoroethylene mold, cured, and vacuum dried at 40-80℃ for 8-24 hours to obtain the final product.

[0009] To further achieve the objectives of this invention, preferably, the monomer A containing two amino groups is an aminopropyl-terminated polydimethylsiloxane or a polyetheramine; the small molecule monomer B containing two aldehyde groups is terephthalaldehyde, o-phthalaldehyde, or glutaraldehyde; and the crosslinking agent C containing three aldehyde groups is pyromellitic methyl ether, 3,4',5-trialdehyde-1,1-biphenyl, or tris(4-aldehyde-biphenyl)amine.

[0010] Further, the organic solvent is one of ethanol, tetrahydrofuran, and N,N-dimethylacetamide; the mass concentration of the crosslinking agent C solution containing three aldehyde groups is 10-40 mg / mL.

[0011] Furthermore, the molar ratio of the monomer A containing two amino groups to the amino group of the adipic acid dihydrazide is 1:0-1:1, and the molar ratio of the small molecule monomer B containing two aldehyde groups to the aldehyde group of the crosslinking agent C is 4:1-0:1.

[0012] Furthermore, the number-average molecular weight of the monomer A containing two amino groups is 600-5000 g / mol.

[0013] The polyimide elastomer obtained by the above preparation method is a polyimide elastomer material that combines high tensile strength, room temperature self-healing and recyclability.

[0014] The recyclability of the polyimide elastomer refers to the process of stirring in a degradation solution at 25-60℃ for 12-48 hours, then placing it in an oven at 60-120℃ for 12-48 hours to remove the degradation solution, and then adding the same type and amount of organic solvent as in the preparation process and stirring for 12-24 hours to obtain the recycled polyimide elastomer.

[0015] Furthermore, the degradation solution refers to a hydrochloric acid solution in ethanol, tetrahydrofuran, or N,N-dimethylacetamide with a molar concentration of 0.1-1 mol / L.

[0016] Compared with the prior art, the present invention has the following advantages and beneficial effects:

[0017] (1) The high tensile, room temperature self-healing and recyclable polyimide elastomer obtained by the present invention has a tensile stress of 0.85-4.56 MPa and an elongation at break of 153-1110%, and a glass transition temperature of -72.6℃ to -45.3℃.

[0018] (2) The high tensile strength, room temperature self-healing and recyclable polyimide elastomer prepared by the present invention benefits from the soft and hard segment structure constructed by the flexible monomer A containing two amino groups and adipic dihydrazide introduced into the structure. The elastomer has advantages such as low glass transition temperature, high tensile stress and high elongation at break.

[0019] (3) The high-tensile, room-temperature self-healing, and recyclable polyimide elastomer network prepared in this invention contains dynamic hydrogen bonds and dynamic imine bonds, exhibiting excellent self-healing properties. After the completely severed elastomer heals at room temperature for 24 hours, the healing efficiency can reach up to 98.3%. Since imine bonds can be rapidly broken in acidic solutions to generate amino and aldehyde groups, the prepared polyimide elastomer can be completely degraded in a 0.1-1 mol / L degradation solution at 25-60℃ for 60-360 minutes. Simultaneously, after completely removing hydrochloric acid by heating, the degraded oligomers and small molecules can regenerate imine bonds, endowing the elastomer with degradable and recyclable properties, realizing the reuse of reaction raw materials. After one degradation-recycling cycle, the elastomer's tensile strength can reach up to 2.07 MPa, and its elongation at break can reach up to 921%. Attached Figure Description

[0020] Figure 1 This is a schematic diagram of the synthesis route for the high-strength, room-temperature self-healing, and recyclable polyimide elastomer prepared in Example 1.

[0021] Figure 2 Photographs of the high-tensile, room-temperature self-healing, and recyclable polyimide elastomer prepared in Example 1 after cutting.

[0022] Figure 3 An optical microscope image of the healing process of the high-tensile, room-temperature self-healing, and recyclable polyimide elastomer prepared in Example 1.

[0023] Figure 4 The image shows a comparison of the high tensile strength, room temperature self-healing and recyclable polyimide elastomer prepared in Example 1 before and after immersion in a 1 mol / L hydrochloric acid-ethanol solution at room temperature for 60 minutes. Detailed Implementation

[0024] To better understand the present invention, the technical solution of the present invention will be further described below with reference to the embodiments and accompanying drawings, but the implementation of the present invention is not limited thereto.

[0025] Example 1

[0026] Figure 1 This is a schematic diagram of the synthesis route for the high-tensile, room-temperature self-healing, and recyclable polyimide elastomer prepared in this embodiment. The specific procedures are as follows:

[0027] 5.0 g of polyetheramine (5 mmol) with a number-average molecular weight of 1000 g / mol and 0.435 g of adipate dihydrazide (2.5 mmol) were mixed at 25 °C and magnetically stirred for 10 min. Then, 0.804 g of terephthalaldehyde (6 mmol) was added, and the reaction was continued with magnetic stirring for 2 h. After the reaction was completed, a linear prepolymer with high viscosity was obtained. 0.1625 g of trimesoaldehyde (1 mmol) dissolved in 10 mL of ethanol was added to the reactor as a crosslinking agent, and the reaction was continued at room temperature for 16 h. After curing in a polytetrafluoroethylene mold, the mixture was vacuum dried at 80 °C for 12 h to obtain a high-tensile, room-temperature self-healing, and recyclable polyimide elastomer.

[0028] According to GB / T 528-2009, the polyimide elastomer prepared in this embodiment was cut and sampled, as follows: Figure 2 As shown, the specimen is dumbbell-shaped, with a standard thickness of 2.0±0.2 mm for the narrow section and a test length of 20.0±0.5 mm. A type 2 cutter was used, with a total length of 75 mm, an end width of 12.5±1.0 mm, a narrow section length of 25.0±1.0 mm, a narrow section width of 4.0±0.1 mm, an outer transition edge radius of 8.0±0.5 mm, and an inner transition edge radius of 12.5±1.0 mm. The cut specimen was used for tensile property testing.

[0029] The glass transition temperature, tensile strength, elongation at break, and healing efficiency of the polyimide elastomer prepared in Example 1 after 24 hours of healing at room temperature are shown in Table 1. As can be seen from Table 1, thanks to the large number of flexible polyetheramine molecular chains in the polymer network, the polyimide elastomer prepared in Example 1 exhibits a glass transition temperature of -52.3℃, a tensile strength of 2.76 MPa, and an elongation at break of 1069%, demonstrating excellent comprehensive mechanical properties. Furthermore, thanks to the synergistic effect of dynamic hydrogen bonds and reversible dynamic imine bonds, the completely severed elastomer showed a healing efficiency of 98.3% after 24 hours of healing at room temperature, indicating that the elastomer possesses good room-temperature self-healing properties. The elastomer was immersed in a 1 mol / L hydrochloric acid-ethanol solution at room temperature for 60 minutes to obtain a homogeneous degradation solution. The degraded solution was then placed in a 120℃ oven for 12 hours to remove hydrochloric acid and ethanol. 10 mL of ethanol was then added and the mixture was stirred for 24 hours to regenerate the recovered polyimide elastomer. The mass loss rate during degradation and the tensile strength and elongation at break after one degradation-recycling cycle are shown in Table 2. As can be seen from Table 2, the remaining mass percentage of the degraded sample was 0%, and the tensile strength and elongation at break were 2.07 MPa and 845%, respectively, indicating that the elastomer has good recyclability.

[0030] Figure 3 Optical microscope images of the healing process of the polyimide elastomer prepared in Example 1. The left image is an optical microscope image of the cut elastomer magnified 200 times, showing that the cut width is about 20 μm; the right image is an optical microscope image of the cut elastomer after healing at room temperature for 24 hours, showing that the cut has almost completely disappeared.

[0031] Figure 4 The comparison image shows the polyimide elastomer prepared in Example 1 before and after immersion in a 1 mol / L hydrochloric acid ethanol solution at room temperature for 60 min. It can be seen that the polyimide elastomer can be completely degraded under the conditions described, with a degradation rate of 100%.

[0032] Example 2

[0033] 50.0 g of aminopropyl-terminated polydimethylsiloxane (10 mmol) with a number-average molecular weight of 5000 g / mol and 1.072 g of phthalaldehyde (8 mmol) were mixed at 25 °C and magnetically stirred for 2 h. After the reaction, a linear prepolymer with high viscosity was obtained. 0.33 g of 3,4',5-trialdehyde-1,1-biphenyl (1.388 mmol) dissolved in 24 mL of tetrahydrofuran solvent was added to the reactor as a crosslinking agent, and the reaction was continued at 40 °C for 24 h. After curing in a polytetrafluoroethylene mold, it was vacuum dried at 40 °C for 24 h to obtain a high-tensile, room-temperature self-healing, and recyclable polyimide elastomer.

[0034] The polyimide elastomer prepared in this embodiment was cut into samples, and the cutting process was the same as in Example 1. The cut sample strips (such as...) Figure 2 It is used for tensile property testing.

[0035] The glass transition temperature, tensile strength, elongation at break, and healing efficiency of the polyimide elastomer prepared in Example 2 after 24 hours of healing at room temperature are shown in Table 1. As can be seen from Table 1, thanks to the large number of flexible polyetheramine molecular chains in the polymer network, the elastomer prepared in this example exhibits a glass transition temperature of -72.6℃, a tensile strength of 0.85 MPa, and an elongation at break of 1110%, demonstrating excellent comprehensive mechanical properties. Furthermore, thanks to the synergistic effect of dynamic hydrogen bonds and reversible dynamic imide bonds, the completely severed elastomer showed a healing efficiency of 97.6% after 24 hours of healing at room temperature, indicating that the elastomer possesses good room-temperature self-healing properties. The elastomer was immersed in a 0.1 mol / L tetrahydrofuran hydrochloride solution at 25℃ for 360 minutes to obtain a homogeneous degraded solution. The degraded solution was then placed in a 60℃ oven for 48 hours to remove hydrochloric acid and tetrahydrofuran. 10 mL of tetrahydrofuran was then added and the mixture was stirred for 12 hours to regenerate the recovered polyimide elastomer. The mass loss rate during the degradation process and the tensile strength and elongation at break after one degradation-recycling cycle are shown in Table 2. As can be seen from Table 2, the remaining mass percentage of the degraded sample was 23.8%, and the tensile strength and elongation at break were 0.63 MPa and 921%, respectively, indicating that the elastomer has good recyclability.

[0036] Optical microscope images of the healing process of the polyimide elastomer prepared in this embodiment and Figure 3 similar.

[0037] Digital photographs of the polyimide elastomer prepared in this example before and after immersion in a 0.1 mol / L tetrahydrofuran hydrochloride solution at 25°C for 360 minutes at room temperature. Figure 4 Similarly, under the stated conditions, the polyimide elastomer was mostly degraded, with only a small amount remaining undegraded.

[0038] Example 3

[0039] 12.0 g of polyetheramine (20 mmol) with a number-average molecular weight of 600 g / mol and 3.48 g of adipate dihydrazide (20 mmol) were mixed at 80 °C and magnetically stirred for 10 min. Then, 3.2 g of glutaraldehyde (32 mmol) was added, and the reaction was continued with magnetic stirring for 6 h. After the reaction was completed, a linear prepolymer with high viscosity was obtained. 3.09 g of tris(4-aldehyde biphenyl)amine (5.55 mmol) dissolved in 50 mL of N,N-dimethylacetamide solvent was added to the reactor as a crosslinking agent, and the reaction was continued at 70 °C for 14 h. After curing in a polytetrafluoroethylene mold, it was vacuum dried at 75 °C for 10 h to obtain a high-tensile, room-temperature self-healing, and recyclable polyimide elastomer.

[0040] The polyimide elastomer prepared in this embodiment was cut into samples, and the cutting process was the same as in Example 1. The cut sample strips (such as...) Figure 2 It is used for tensile property testing.

[0041] The glass transition temperature, tensile strength, elongation at break, and healing efficiency of the polyimide elastomer prepared in Example 3 after 24 hours of healing at room temperature are shown in Table 1. As can be seen from Table 1, thanks to the large number of flexible polyetheramine molecular chains in the polymer network, the elastomer prepared in Example 3 exhibits a glass transition temperature of -45.3℃, a tensile strength of 4.56 MPa, and an elongation at break of 153%, demonstrating excellent comprehensive mechanical properties. Furthermore, thanks to the synergistic effect of dynamic hydrogen bonds and reversible dynamic imide bonds, the completely severed elastomer showed a healing efficiency of 86.7% after 24 hours of healing at room temperature, indicating that the elastomer possesses good room-temperature self-healing properties. The elastomer was immersed in a 0.5 mol / L N,N-dimethylacetamide hydrochloride solution at 60℃ for 300 minutes to obtain a homogeneous degraded solution. The degraded solution was then placed in an 80℃ oven for 24 hours to remove hydrochloric acid and N,N-dimethylacetamide. 10 mL of N,N-dimethylacetamide was then added and the mixture was stirred for 16 hours to regenerate the recovered polyimide elastomer. The mass loss rate during the degradation process and the tensile strength and elongation at break after one degradation-recycling cycle are shown in Table 2. As can be seen from Table 2, the remaining mass percentage of the degraded sample was 5.6%, and the tensile strength and elongation at break were 3.27 MPa and 89%, respectively, indicating that the elastomer has good recyclability.

[0042] Optical microscope images of the healing process of the polyimide elastomer prepared in this embodiment and Figure 3 similar.

[0043] Digital photographs of the polyimide elastomer prepared in this example before and after immersion in a 0.5 mol / L N,N-dimethylacetamide hydrochloride solution at 60°C for 300 minutes at room temperature. Figure 4Similarly, under the stated conditions, the polyimide elastomer was mostly degraded, with only a small amount remaining undegraded.

[0044] Example 4

[0045] 15.0 g of polyetheramine (5 mmol) with a number average molecular weight of 3000 g / mol and 0.435 g of adipate dihydrazide (2.5 mmol) were mixed at 40 °C and magnetically stirred for 10 min. Then, 2.79 g of tris(4-aldehyde biphenyl)amine (5 mmol) dissolved in 5 mL of ethanol solvent was added to the reactor as a crosslinking agent. The reaction was continued at 80 °C for 14 h. After curing in a polytetrafluoroethylene mold, the product was vacuum dried at 60 °C for 16 h to obtain a high tensile strength, room temperature self-healing and recyclable polyimide elastomer.

[0046] The polyimide elastomer prepared in this embodiment was cut into samples, and the cutting process was the same as in Example 1. The cut sample strips (such as...) Figure 2 It is used for tensile property testing.

[0047] The glass transition temperature, tensile strength, elongation at break, and healing efficiency of the polyimide elastomer prepared in Example 4 after 24 hours of healing at room temperature are shown in Table 1. As can be seen from Table 1, thanks to the large number of flexible polyetheramine molecular chains in the polymer network, the elastomer prepared in Example 4 exhibits a glass transition temperature of -51.2℃, a tensile strength of 2.32 MPa, and an elongation at break of 834%, demonstrating excellent comprehensive mechanical properties. Furthermore, thanks to the synergistic effect of dynamic hydrogen bonds and reversible dynamic imide bonds, the completely severed elastomer showed a healing efficiency of 83.4% after 24 hours of healing at room temperature, indicating that the elastomer possesses good room-temperature self-healing properties. The elastomer was immersed in a 0.2 mol / L hydrochloric acid-ethanol solution at 50℃ for 180 minutes to obtain a homogeneous degradation solution. The degraded solution was then placed in a 100℃ oven for 20 hours to remove hydrochloric acid and ethanol. 10 mL of ethanol was then added and the mixture was stirred for 22 hours to regenerate the recovered polyimide elastomer. The mass loss rate during the degradation process and the tensile strength and elongation at break after one degradation-recycling cycle are shown in Table 2. As can be seen from Table 2, the remaining mass percentage of the degraded sample was 12.9%, and the tensile strength and elongation at break were 1.93 MPa and 756%, respectively, indicating that the elastomer has good recyclability.

[0048] Optical microscope images of the healing process of the polyimide elastomer prepared in this embodiment and Figure 3 similar.

[0049] Digital photographs of the polyimide elastomer prepared in this example before and after immersion in a 0.2 mol / L hydrochloric acid-ethanol solution at 50°C for 180 minutes at room temperature. Figure 4Similarly, under the stated conditions, the polyimide elastomer was mostly degraded, with only a small amount remaining undegraded.

[0050] Table 1 shows the glass transition temperature, tensile strength, elongation at break, and healing efficiency of the high-tensile, room-temperature self-healing, and recyclable polyimide elastomer strips prepared in Examples 1-4 of this invention. The glass transition temperature was measured using differential scanning calorimetry, with the temperature increased from -100℃ to 90℃ at a rate of 10℃ / min. Tensile strength and elongation at break were obtained through tensile testing according to GB / T528-2009. The healing efficiency was calculated according to the following formula:

[0051]

[0052] Table 2 shows the residual mass ratio of the high tensile strength, room temperature self-healing, and recyclable polyimide elastomers prepared in Examples 1-4 of this invention after degradation, and the data on tensile strength and elongation at break after one degradation-recycling cycle; wherein, the tensile strength and elongation at break of the samples after one degradation-recycling cycle were obtained by tensile testing according to GB / T 528-2009; the residual mass ratio of the degraded samples was calculated according to the following formula 2:

[0053]

[0054] Table 1

[0055]

[0056] Table 2

[0057]

[0058] The above embodiments are preferred embodiments of the present invention, but the embodiments of the present invention are not limited to the above embodiments. Any changes, modifications, substitutions, combinations, or simplifications made without departing from the spirit and principle of the present invention shall be considered equivalent substitutions and shall be included within the protection scope of the present invention.

Claims

1. A method for preparing a high-tensile, room-temperature self-healing, and recyclable polyimide elastomer, characterized in that: Specifically, the preparation steps include the following: A monomer A containing two amino groups, a small molecule monomer B containing two aldehyde groups, and adipic acid dihydrazide are condensed to generate a linear macromolecular prepolymer containing dynamic imine bonds and hydrazide bonds; then a crosslinking agent C containing three aldehyde groups is added to carry out a crosslinking reaction; finally, the reactants are poured into a polytetrafluoroethylene mold, cured, and vacuum dried to obtain the target product. The monomer A containing two amino groups is an aminopropyl-terminated polydimethylsiloxane or a polyetheramine; The molar ratio of the monomer A containing two amino groups to the amino group of adipic acid dihydrazide is 1:0-1:1; the molar ratio of the small molecule monomer B containing two aldehyde groups to the aldehyde group of the crosslinking agent C is 4:1-0:

1.

2. The method for preparing the high-tensile, room-temperature self-healing, and recyclable polyimide elastomer according to claim 1, characterized in that: The small molecule monomer B containing two aldehyde groups is terephthalaldehyde, o-phthalaldehyde, or glutaraldehyde; the crosslinking agent C containing three aldehyde groups is pyromellitic methyl methacrylate, 3,4',5-trialdehyde-1,1-biphenyl, or tri(4-aldehyde-biphenyl)amine.

3. The method for preparing the high-tensile, room-temperature self-healing, and recyclable polyimide elastomer according to claim 1, characterized in that: The crosslinking agent C solution containing three aldehyde groups refers to a solution formed by dissolving crosslinking agent C in one of ethanol, tetrahydrofuran, and N,N-dimethylacetamide; the mass concentration of the crosslinking agent C solution containing three aldehyde groups is 10-40 mg / mL.

4. The method for preparing the high-tensile, room-temperature self-healing, and recyclable polyimide elastomer according to claim 1, characterized in that: The number-average molecular weight of monomer A containing two amino groups is 600-5000 g / mol.

5. The method for preparing the high-tensile, room-temperature self-healing, and recyclable polyimide elastomer according to claim 1, characterized in that: The condensation reaction is carried out at 25-80℃ for 2-6 hours.

6. The method for preparing the high-tensile, room-temperature self-healing, and recyclable polyimide elastomer according to claim 1, characterized in that: The crosslinking reaction is performed at 25-80℃ for 12-24 hours.

7. The method for preparing the high-tensile, room-temperature self-healing, and recyclable polyimide elastomer according to claim 1, characterized in that: The vacuum drying temperature is 40-80℃, and the drying time is 8-24h.

8. A high-tensile, room-temperature self-healing, and recyclable polyimide elastomer obtained by the preparation method according to any one of claims 1-7.

9. The high-tensile, room-temperature self-healing, and recyclable polyimide elastomer according to claim 8, characterized in that: The recyclability of polyimide elastomer refers to the process of stirring the polyimide elastomer in a degradation solution at 25-60℃ for 12-48 hours, then placing it in an oven at 60-120℃ for 12-48 hours to remove the degradation solution, and then adding the same type and amount of organic solvent as in the preparation process and stirring for 12-24 hours to obtain the recovered polyimide elastomer; the degradation solution refers to a solution of hydrochloric acid in ethanol, tetrahydrofuran, or N,N-dimethylacetamide with a molar concentration of 0.1-1 mol / L.

Citation Information

Patent Citations

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