A hydrogen bond-shiff base dual self-healing lithium single-ion polymer electrolyte with self-healing ability, a preparation method and application thereof
By using a hydrogen bond-Schiff base dual self-healing lithium single-ion polymer electrolyte, the problem of the inability of traditional polymer electrolytes to self-repair has been solved, realizing the self-healing of lithium batteries and the suppression of lithium dendrites, improving battery performance and lifespan, and reducing costs.
Patent Information
- Authority / Receiving Office
- CN · China
- Patent Type
- Patents(China)
- Current Assignee / Owner
- SUN YAT SEN UNIV
- Filing Date
- 2023-12-08
- Publication Date
- 2026-06-26
AI Technical Summary
Traditional polymer electrolytes cannot repair the minute damage inside the battery, causing the lithium battery to degrade in performance during cycling and eventually lose its ability to work. Furthermore, the formation of lithium dendrites is difficult to suppress.
A hydrogen-Schiff base dual self-healing lithium single-ion polymer electrolyte is adopted. Hydrogen bonds and Schiff base bonds are introduced through copolymerization to endow the polymer with self-healing ability, fix lithium ions, and inhibit the formation of lithium dendrites.
It improves the cycle performance of lithium batteries, extends battery life, reduces costs, and simplifies the processing, making it suitable for industrial production.
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Figure CN117659301B_ABST
Abstract
Description
Technical Field
[0001] This invention relates to the field of lithium-ion batteries, and specifically to a method for preparing a hydrogen-bonded-Schiff base dual self-healing lithium single-ion polymer electrolyte with self-healing capabilities. Background Technology
[0002] During operation, lithium batteries are susceptible to malfunctions caused by external forces, dendrite formation, breakage of the solid-electrolyte interface / intermediate phase (SEI) and cathode electrolyte interface (CEI), gas release, and short circuits. Traditional polymer electrolytes lack self-repair capabilities, meaning that even minor internal damage cannot be repaired promptly. This leads to a continuous decline in battery performance during cycling, ultimately resulting in the battery losing its ability to function.
[0003] Traditional polymer electrolytes achieve ion conduction through the addition of lithium salts. In these electrolytes, both lithium ions and their corresponding anions are mobile. During battery discharge cycles, Li+ ions and counter anions move in opposite directions within the polymer matrix. Because the electrodes block the anions, they tend to accumulate on the anode side, leading to a concentration gradient and concentration polarization. This makes lithium dendrites more likely to form in the battery, ultimately causing it to cease operation.
[0004] Self-healing polymers are polymers that, under certain conditions, can self-repair some or all of their properties after being damaged. Based on the self-healing mechanism, self-healing polymers can be divided into external self-healing (repaired by external repair agents) and internal self-healing (repaired through reversible chemical bonds). Internal self-healing can be further divided into reversible covalent and non-covalent bonds based on the reversible chemical bonds involved. Polymers with reversible covalent bonds often require external stimulation for repair due to the high bond energy of the covalent bonds. Therefore, how to endow polymer electrolytes with self-healing capabilities to promptly repair minor damage in the electrolyte, extend battery life, and improve operating time remains an important research topic. Summary of the Invention
[0005] The purpose of this invention is to construct a hydrogen-bonded-Schiff base dual self-healing lithium single-ion polymer electrolyte system with self-healing capabilities. This system can repair damage generated in the electrolyte during lithium battery use and inhibit the formation of lithium dendrites, thereby improving the cycle performance of lithium batteries. Based on this, this invention provides a hydrogen-bonded-Schiff base dual self-healing lithium single-ion polymer electrolyte with self-healing capabilities, its preparation method, and its applications.
[0006] To achieve the above objectives, the present invention provides a method for preparing a hydrogen-bonded-Schiff base dual self-healing lithium single-ion polymer electrolyte with self-healing capabilities, comprising the following steps:
[0007] 1) Using N,N-dimethylformamide as solvent and azobisisobutyronitrile as initiator, melamine-modified monomers containing hydrogen bonds and amino groups were mixed as self-healing functional group donors, polyethylene glycol methyl ether methacrylate as ion-conducting group donors, and lithium 4-styrenesulfonyl (benzenesulfonyl)imide as lithium ion donors, and copolymerized under argon protection atmosphere and heating conditions of 50-80℃ to obtain copolymers;
[0008] The structural formula of the melamine-modified monomer containing hydrogen bonds and amino groups is as follows:
[0009]
[0010] In the formula, R4 is a methyl, ethyl, propyl, or butyl group, etc.
[0011] 2) Dissolve the copolymer obtained in step 1) and a small molecule compound with multiple (two or more) aldehyde groups in an organic solvent. After removing the solvent, carry out a Schiff base reaction under high temperature vacuum conditions of 100℃~120℃ to obtain a hydrogen bond-Schiff base dual self-healing lithium single ion polymer electrolyte with self-healing ability.
[0012] As a further preferred embodiment of the present invention, the method for preparing the melamine-modified monomer containing hydrogen bonds and amino groups includes the following steps:
[0013] Using dimethyl sulfoxide as solvent, R4-based isocyanate and melamine were mixed and reacted at 110℃±2℃. After the reaction was completed, the product was precipitated with ice water to obtain N-R4-N'-(4,6-diamino-1,3,5-triazin-2-yl)urea, wherein R4-based is a methyl, ethyl, propyl or butyl group.
[0014] N-R4-N'-(4,6-diamino-1,3,5-triazin-2-yl)urea and isocyanate methacrylate were added to pyridine, and nitrobenzene was added dropwise. The mixture was heated and stirred at 80-95°C for 6-24 hours. The insoluble matter was then filtered out and crystallized by adding water. The resulting solid was a melamine-modified monomer containing hydrogen bonds and amino groups.
[0015] As a further preferred embodiment of the present invention, the molecular weight of the polyethylene glycol methyl ether methacrylate is 400 to 1200.
[0016] As a further preferred technical solution of the present invention, in the copolymerization reaction of step 1), the molar ratio of melamine-modified monomer, polyethylene glycol methyl ether methacrylate, and lithium 4-styrenesulfonyl (benzenesulfonyl)imide is 1:5:1-5.
[0017] As a further preferred embodiment of the present invention, the small molecule compound with multiple aldehyde groups is terephthalaldehyde or pyromellitic terephthalaldehyde.
[0018] As a further preferred technical solution of the present invention, the molar ratio of amino groups in the melamine-modified monomer to aldehyde groups in the small molecule compound with multiple aldehyde groups is 1:1.
[0019] According to another aspect of the present invention, the present invention also provides a hydrogen-bonded-Schiff base dual self-healing lithium single-ion polymer electrolyte with self-healing capability, which is prepared by the above method.
[0020] According to another aspect of the present invention, the present invention also provides the application of a hydrogen-bonded-Schiff base dual self-healing lithium single-ion polymer electrolyte with self-healing capability in lithium batteries.
[0021] Compared with the prior art, the present invention has the following beneficial technical effects:
[0022] 1) The preparation method of the present invention constructs a hydrogen bond-Schiff base dual self-healing lithium single-ion polymer electrolyte system with good mechanical properties and certain self-healing ability. When applied to lithium batteries, it can improve the cycle performance of lithium batteries.
[0023] 2) Since lithium salts are extremely hygroscopic, and some lithium salts decompose when exposed to water, they often need to be handled in a glove box. However, the hydrogen bond-Schiff base dual self-healing lithium single-ion polymer electrolyte system constructed in this invention does not require the addition of external lithium salts, resulting in lower costs. It is also easy to process and has the ability to conduct lithium ions. At the same time, it can suppress the formation of lithium dendrites and improve the cycle performance of lithium batteries.
[0024] 3) The preparation method of the present invention uses raw materials that are inexpensive, have low risk and are widely available. At the same time, the reaction conditions of the present invention are relatively mild, easy to control, simple to operate and easy to realize industrial production. Attached Figure Description
[0025] The present invention will now be described in further detail with reference to the accompanying drawings and specific embodiments.
[0026] Figure 1 This is the general reaction formula for the copolymerization reaction of butyl-triazine-MA, polyethylene glycol methyl ether methacrylate and lithium 4-styrenesulfonyl (benzenesulfonyl)imide in Example 1.
[0027] Figure 2This is the general reaction formula for the reaction of the copolymer obtained in Example 1 with the small molecule aldehyde compound p-phenylenedialdehyde.
[0028] Figure 3 The thermogravimetric curves of the copolymer and polymer electrolyte obtained in Example 1 are shown.
[0029] Figure 4 The 1H NMR spectrum of butyl-triazine-MA in Example 1 is shown.
[0030] Figure 5 The image shows the 1H NMR spectrum of the copolymer in Example 1.
[0031] Figure 6 The two curves in the figure are the stretching curves of the polymer electrolyte membrane obtained in Example 1 when stretched at a stretching rate of 10 mm / min.
[0032] Figure 7 The graph shows the constant current charge-discharge cycle of a lithium battery at a current density of 0.1 mA / cm², obtained by assembling the polymer electrolyte membrane obtained in Example 1 in the order of lithium sheet-polymer membrane-lithium sheet and performing constant current charge-discharge.
[0033] The objectives, features, and advantages of this invention will be further explained in conjunction with the embodiments and with reference to the accompanying drawings. Detailed Implementation
[0034] The specific embodiments of the present invention will be described in detail below with reference to the accompanying drawings. It should be understood that the specific embodiments described herein are for illustration and explanation only and are not intended to limit the present invention.
[0035] Unless otherwise defined, the technical terms used in the following embodiments have the same meanings as commonly understood by those skilled in the art to which this invention pertains. Unless otherwise specified, the experimental reagents used in the following embodiments are conventional biochemical reagents; and the experimental methods described are conventional methods.
[0036] This invention endows the polymer electrolyte with self-healing capabilities by introducing hydrogen bonds and Schiff base bonds, enabling it to promptly repair minor damage in the electrolyte and extend battery life, resulting in longer operating times. In addition to self-healing capabilities, the lithium single-ion polymer electrolyte of this invention can immobilize anions in the lithium salt through various methods, preventing them from moving during charge and discharge. Specifically, lithium ions are introduced into the polymer chain through polymer synthesis. During lithium ion dissociation, because the anions are directly connected to the polymer chain and cannot move, the ion transference number can approach 1, resulting in better cycle performance.
[0037] Example 1
[0038] Step 1: Synthesis of melamine-modified monomer containing hydrogen bonds and amino groups (hereinafter referred to as R4-triazine-MA). In this example, R4 = butyl:
[0039] A solution of 15.5 g (0.1 mol) of isocyanate in 10 mL of DMSO was added dropwise to a stirred slurry of 12.6 g (0.1 mol) of melamine in 50 mL of DMSO over 0.5 hours at 110 °C ± 2 °C. In almost all cases, the reaction temperature increased by a few degrees. After the addition of isocyanate, the reaction mixture was maintained at 110 °C ± 2 °C for 6 hours, followed by precipitation with ice water to obtain N-butyl-N'-(4,6-diamino-1,3,5-triazin-2-yl)urea. The product was recrystallized from DMF.
[0040] 22.5 g of N-butyl-N'-(4,6-diamino-1,3,5-triazin-2-yl)urea and 15.5 g of isocyanate methacrylate were added to 400 mL of pyridine, along with 1 drop of nitrobenzene. The mixture was heated and stirred at 90 °C for 12 hours. The insoluble matter was filtered off, and crystallization was carried out by adding 2 L of water. The resulting solid was filtered off, washed with water, and dried under reduced pressure. 19.8 g of a melamine-modified monomer containing hydrogen bonds and amino groups, namely butyl-triazine-MA, was synthesized; it was a cream-colored solid.
[0041] Step 2: Dissolve 0.76 g (2 mmol) butyl-triazine-MA (molecular weight 380), 4.75 g (10 mmol) polyethylene glycol methyl ether methacrylate (molecular weight approximately 475), and 2.48 g (7.5 mmol) lithium 4-styrenesulfonyl (benzenesulfonyl)imide in 20 ml DMF, then add 3.20 mg (0.195 mmol) azobisisobutyronitrile (AIBN), and react at 70 °C under argon protection for 1 day. The reactants precipitate in ice-cold diethyl ether to obtain a copolymer, which is then dried in a vacuum oven at 80 °C. At this point, the molar ratio of melamine-modified monomer: polyethylene glycol methyl ether methacrylate: lithium 4-styrenesulfonyl (benzenesulfonyl)imide in the copolymer is 1:5:3.75.
[0042] Step 3: Take 1g of the dried copolymer, dissolve it in 2mL of N,N-dimethylacetamide, add 0.0168g of terephthalaldehyde, pour it into a polytetrafluoroethylene mold, dry it in a vacuum oven at 80℃ for 1 day to remove the solvent, and then react it in a vacuum oven at 120℃ for 1 day to obtain a hydrogen bond-Schiff base dual self-healing lithium single ion polymer electrolyte (hereinafter referred to as polymer electrolyte) membrane with self-healing ability.
[0043] Figure 1 This is the general reaction formula for the copolymerization reaction of butyl-triazine-MA, polyethylene glycol methyl ether methacrylate and lithium 4-styrenesulfonyl (benzenesulfonyl)imide in Example 1.
[0044] Figure 2 This is the general reaction formula for the reaction of the copolymer obtained in Example 1 with the small molecule aldehyde compound p-phenylenedialdehyde.
[0045] Figure 3 The thermogravimetric curves of the copolymer and polymer electrolyte obtained in Example 1 are shown in the attached figure. Figure 3 The results show that the weight loss curves of the two are basically the same, with two main weight loss stages. Due to the strong water absorption of PEG, the first weight loss stage is the stage of polymer water loss, and the second stage is the stage of cross-linked polymer degradation, starting from 220℃ and ending at 420℃, with a weight loss rate of 79%. The thermogravimetric curves show that the polymer electrolyte has good thermal stability and only decomposes at 220℃, which meets the requirements for lithium battery use.
[0046] Figure 4 The image shows the 1H NMR spectrum of butyl-triazine-MA in Example 1, where the peak at 0.90 ppm corresponds to the hydrogen atom on the butyl group, and the peak at 6.66 ppm corresponds to the amino group attached to the triazine group.
[0047] Figure 5 The NMR spectrum of the copolymer in Example 1 is shown below. Figure 4 By comparing the peaks that yield triazine and butyl groups, the occurrence of the copolymerization reaction can be determined.
[0048] Figure 6 The two curves shown are, respectively, the tensile curve obtained by stretching the polymer electrolyte membrane obtained in Example 1 at a stretching rate of 10 mm / min, and the tensile curve obtained by completely cutting the polymer electrolyte membrane with a knife, repairing it at 60°C for 24 hours, and then stretching it at the same stretching rate. It can be seen that the mechanical properties of the initial polymer electrolyte membrane and the repaired polymer electrolyte membrane are similar, which confirms that the obtained polymer electrolyte has self-healing properties.
[0049] Figure 7 The graph shows the constant current charge-discharge cycle of the lithium battery obtained in Example 1, which was assembled with the polymer electrolyte membrane in the order of lithium sheet-polymer membrane-lithium sheet, at a current density of 0.1 mA / cm2. It can be seen that the assembled battery has good cycle performance.
[0050] Example 2
[0051] The steps for preparing the melamine-modified monomer containing hydrogen bonds and amino groups in Example 2 are the same as in Example 1, except that the starting reactant is methyl isocyanate and the product is methyl-triazine-MA.
[0052] 0.68 g (2 mmol) of methyl-triazine-MA (molecular weight 338), 4.75 g (10 mmol) of polyethylene glycol methyl ether methacrylate (molecular weight approximately 475), and 2.48 g (7.5 mmol) of lithium 4-styrenesulfonyl (benzenesulfonyl)imide were dissolved in 20 ml of DMF. Then, 3.20 mg (0.195 mmol) of azobisisobutyronitrile was added, and the mixture was reacted at 70 °C under argon protection for 1 day. The reactants precipitated in ice-cold diethyl ether and were then dried in a vacuum oven at 80 °C. At this point, the molar ratio of modified melamine monomer: polyethylene glycol methyl ether methacrylate: lithium 4-styrenesulfonyl (benzenesulfonyl)imide in the copolymer was 1:5:3.75.
[0053] Take 1g of the dried copolymer from the previous step, dissolve it in 2mL of N,N-dimethylacetamide, then add 0.0169g of terephthalaldehyde, pour the mixture into a polytetrafluoroethylene mold, dry it in a vacuum oven at 80℃ for 1 day to remove the solvent, and then react it in a vacuum oven at 120℃ for 1 day to obtain a polymer electrolyte membrane. Referring to Example 1, the mechanical properties, self-healing ability, and electrochemical performance of the polymer electrolyte membrane of Example 2 were tested. The results showed that there was no significant difference in properties between the polymer electrolyte membranes obtained in Example 2 and Example 1; their mechanical properties, self-healing ability, and electrochemical performance were the same.
[0054] Example 3
[0055] The steps for preparing the melamine-modified monomer containing hydrogen bonds and amino groups in Example 3 are the same as those in Example 1, except that the starting reactant is butyl isocyanate and the product is butyl-triazine-MA.
[0056] 0.76 g (2 mmol) of butyl-triazine-MA (molecular weight 380), 12.00 g (10 mmol) of polyethylene glycol methyl ether methacrylate (molecular weight approximately 1200), and 2.48 g (7.5 mmol) of lithium 4-styrenesulfonyl (benzenesulfonyl)imide were dissolved in 20 ml of DMF. Then, 3.20 mg (0.195 mmol) of azobisisobutyronitrile was added, and the mixture was reacted at 70 °C under argon protection for 1 day. The reactants precipitated in ice-cold diethyl ether and were then dried in a vacuum oven at 80 °C. At this point, the molar ratio of modified melamine monomer: polyethylene glycol methyl ether methacrylate: lithium 4-styrenesulfonyl (benzenesulfonyl)imide in the copolymer was 1:5:3.75.
[0057] Take 1g of the dried copolymer from the previous step, dissolve it in 2mL of N,N-dimethylacetamide, add 0.0048g of terephthalaldehyde, pour it into a polytetrafluoroethylene mold, dry it in a vacuum oven at 80℃ for 1 day to remove the solvent, and then react it in a vacuum oven at 120℃ for 1 day to obtain a polymer electrolyte membrane. Referring to Example 1, the mechanical properties, self-healing ability, and electrochemical performance of the polymer electrolyte membrane of Example 3 were tested. The results showed that compared with the polymer electrolyte membrane obtained in Example 1, the mechanical properties of Example 3 were worse, but it still had fairly good self-healing performance (but worse than that of Example 1). This is because the number of hydrogen bonds in the polymer matrix decreased. However, the impedance of the battery assembled with it was lower, and the cycle performance of the assembled battery was also better.
[0058] Example 4
[0059] 0.76 g (2 mmol) of butyl-triazine-MA (molecular weight 380), 4.75 g (10 mmol) of polyethylene glycol methyl ether methacrylate (molecular weight approximately 475), and 0.66 g (2 mmol) of lithium 4-styrenesulfonyl (benzenesulfonyl)imide were dissolved in 20 ml of DMF. Then, 2.30 mg (0.140 mmol) of azobisisobutyronitrile was added, and the mixture was reacted at 70 °C under argon protection for 1 day. The reactants precipitated in ice-cold diethyl ether and were then dried in a vacuum oven at 80 °C. At this point, the molar ratio of modified melamine monomer: polyethylene glycol methyl ether methacrylate: lithium 4-styrenesulfonyl (benzenesulfonyl)imide in the copolymer was 1:5:1.
[0060] Take 1g of the dried copolymer from the previous step, dissolve it in 2mL of N,N-dimethylacetamide, then add 0.0176g of terephthalaldehyde, pour the mixture into a polytetrafluoroethylene mold, dry it in a vacuum oven at 80℃ for 1 day to remove the solvent, and then react it in a vacuum oven at 120℃ for 1 day to obtain the polymer electrolyte membrane. Referring to Example 1, the mechanical properties, self-healing ability, and electrochemical performance of the polymer electrolyte membrane of Example 4 were tested. The results showed that compared with the polymer electrolyte membrane obtained in Example 1, the polymer electrolyte membrane of Example 4 had worse mechanical properties, but stronger self-healing ability, and the assembled battery had better cycle performance.
[0061] Comparative Example 1
[0062] This comparative example serves as a comparison experiment with Example 1. The difference in preparation method between this example and Example 1 is that butyl-triazine-MA is not added during the copolymerization reaction; the rest of the preparation method is the same as in Example 1. This preparation method cannot yield a polymer electrolyte membrane; it only yields a viscous liquid.
[0063] Comparative Example 2
[0064] This comparative example serves as a comparison experiment with Example 1. The difference in preparation method between this example and Example 1 is that lithium 4-styrenesulfonyl (benzenesulfonyl)imide is not added during the copolymerization reaction. Instead, lithium bis(trifluoromethanesulfonyl)imide is added in the corresponding molar amount after dissolving the copolymer with N,N-dimethylformamide. The remaining preparation methods are the same as in Example 1. Testing showed that the polymer electrolyte membrane obtained by this method has poor mechanical properties, and the cycle performance of the assembled battery is far inferior to that of Example 1.
[0065] Comparative Example 3
[0066] This comparative example serves as a comparison experiment with Example 1. The difference in preparation method between this example and Example 1 is that no small molecule compound containing multiple aldehyde groups is added; the rest of the preparation method is the same as in Example 1. Testing revealed that the polymer membrane obtained by this preparation method has poor mechanical properties. Batteries using this polymer electrolyte membrane as the electrolyte exhibit reduced suppression of lithium dendrites and significantly worsened cycle performance.
[0067] While specific embodiments of the present invention have been described above, those skilled in the art should understand that these are merely illustrative examples, and various changes or modifications can be made to these embodiments without departing from the principles and essence of the present invention. The scope of protection of the present invention is defined only by the appended claims.
Claims
1. A method for preparing a hydrogen-bonded-Schiff base dual self-healing lithium single-ion polymer electrolyte with self-healing capabilities, characterized in that, Includes the following steps: 1) Using N,N-dimethylformamide as solvent and azobisisobutyronitrile as initiator, melamine-modified monomers containing hydrogen bonds and amino groups were mixed as self-healing functional group donors, polyethylene glycol methyl ether methacrylate as ion-conducting group donors, and lithium 4-styrenesulfonyl (benzenesulfonyl)imide as lithium ion donors and copolymerized under heating conditions to obtain a copolymer; The structural formula of the melamine-modified monomer containing hydrogen bonds and amino groups is as follows: In the formula, R4 is methyl, ethyl, propyl or butyl; 2) The copolymer obtained in step 1) and the small molecule compound with multiple aldehyde groups are dissolved in an organic solvent. After removing the solvent, a Schiff base reaction is carried out under high temperature vacuum conditions of 100℃~120℃ to obtain a hydrogen bond-Schiff base dual self-healing lithium single ion polymer electrolyte with self-healing ability.
2. The method for preparing the hydrogen-bonded-Schiff base dual self-healing lithium single-ion polymer electrolyte with self-healing capability according to claim 1, characterized in that, The method for preparing the melamine-modified monomer containing hydrogen bonds and amino groups includes the following steps: Using dimethyl sulfoxide as solvent, R4-based isocyanate and melamine were mixed and reacted at 110℃±2℃. After the reaction was completed, the product was precipitated with ice water to obtain N-R4-N'-(4,6-diamino-1,3,5-triazin-2-yl)urea, wherein R4-based is a methyl, ethyl, propyl or butyl group. N-R4-N'-(4,6-diamino-1,3,5-triazin-2-yl)urea and isocyanate methacrylate were added to pyridine, nitrobenzene was added dropwise, and the mixture was heated and stirred at 80-95℃. The insoluble matter was then filtered out and crystallized by adding water. The resulting solid was a melamine-modified monomer containing hydrogen bonds and amino groups.
3. The method for preparing the hydrogen-bonded-Schiff base dual self-healing lithium single-ion polymer electrolyte with self-healing capability according to claim 1, characterized in that, The molecular weight of the polyethylene glycol methyl ether methacrylate is 400 to 1200.
4. The method for preparing the hydrogen-bonded-Schiff base dual self-healing lithium single-ion polymer electrolyte with self-healing capability according to claim 1, characterized in that, In the copolymerization reaction of step 1), the molar ratio of melamine-modified monomer, polyethylene glycol methyl ether methacrylate, and lithium 4-styrenesulfonyl (benzenesulfonyl)imide is 1:5:1-5.
5. The method for preparing the hydrogen-bonded-Schiff base dual self-healing lithium single-ion polymer electrolyte with self-healing capability according to claim 1, characterized in that, In step 1), the copolymerization temperature under heating conditions is 50-80℃.
6. The method for preparing the hydrogen-bonded-Schiff base dual self-healing lithium single-ion polymer electrolyte with self-healing capability according to claim 1, characterized in that, In step 1), an argon protective atmosphere is used during copolymerization under heating conditions.
7. The method for preparing the hydrogen-bonded-Schiff base dual self-healing lithium single-ion polymer electrolyte with self-healing capability according to claim 1, characterized in that, The small molecule compound with multiple aldehyde groups is terephthalaldehyde or pyromellitic terephthalaldehyde.
8. The method for preparing the hydrogen-bonded-Schiff base dual self-healing lithium single-ion polymer electrolyte with self-healing capability according to any one of claims 1-7, characterized in that, The molar ratio of amino groups in melamine-modified monomers to aldehyde groups in small molecule compounds with multiple aldehyde groups is 1:
1.
9. A hydrogen-bonded-Schiff base dual self-healing lithium single-ion polymer electrolyte with self-healing capabilities, characterized in that, Prepared by the method described in any one of claims 1-8.
10. The application of the hydrogen-bonded-Schiff base dual self-healing lithium single-ion polymer electrolyte with self-healing capability as described in claim 9 in lithium batteries.