High-transference number solid electrolyte with high-strength and high-toughness semi-interpenetrating network structure and preparation method and application of high-transference number solid electrolyte
By using a solid electrolyte with a high-strength and high-toughness semi-interpenetrating network structure, the problems of insufficient mechanical strength and low ionic conductivity of polymer matrix are solved, enabling the application of lithium battery materials with high safety and high energy density.
Patent Information
- Application Number
- CN202511451190.3
- Authority / Receiving Office
- CN · China
- Patent Type
- Applications(China)
- Current Assignee / Owner
- Filing Date
- 2025-10-11
- Publication Date
- 2025-12-30
AI Technical Summary
Existing polymer-based solid electrolytes have insufficient mechanical strength, are easily punctured by lithium dendrites, have low ionic conductivity, and poor interfacial compatibility, resulting in insufficient safety and electrochemical stability.
A solid electrolyte employing a high-strength and high-toughness semi-interpenetrating network structure is formed by combining sulfonated high ion-conducting self-contained microporous polymers with linear polymers to create a semi-interpenetrating network structure that combines rigidity and flexibility. Continuous and uniform interconnected microporous channels are formed between molecular chains, which synergistically regulate the interaction between lithium ions and solvents.
It improves the ionic conductivity and lithium-ion transference number of solid electrolytes, suppresses lithium dendrite formation, reduces interface impedance, enhances battery cycle stability, and provides support for high-safety and high-energy-density lithium battery materials.
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Figure CN121237993A_ABST
Abstract
Description
Technical Field
[0001] This invention belongs to the field of solid-state lithium battery technology, specifically relating to a high-mobility-number solid electrolyte with a high-strength and high-toughness semi-interpenetrating network structure, its preparation method, and its application. Background Technology
[0002] Lithium-ion batteries have become important electrochemical energy storage devices due to their high energy density, high charge-discharge rate, and long cycle life. However, traditional liquid electrolytes suffer from problems such as low flash point and flammability. Thermal runaway can lead to fires, explosions, and the release of toxic gases, posing serious safety hazards. Therefore, developing solid-state electrolytes with high safety, high mechanical strength, and electrochemical stability has become a key research focus.
[0003] Polymer solid electrolytes have attracted much attention due to their advantages such as ease of synthesis, lightweight, low cost, and wide electrochemical window. However, their low ionic conductivity and insufficient mechanical strength limit their commercial application. Existing polymer matrices are mostly linear polymers, such as PVDF-HFP, PEO, and PMMA, which have poor mechanical strength and are easily pierced by lithium dendrites. Meanwhile, self-polymerizing microporous polymers are too rigid, resulting in low ionic conductivity and poor interfacial compatibility. Therefore, there is an urgent need to develop novel solid electrolyte materials that combine high ionic conductivity, excellent mechanical properties, and good interfacial stability. Summary of the Invention
[0004] To overcome the problems existing in the prior art, the present invention provides a high mobility number solid electrolyte with a high-strength and high-toughness semi-interpenetrating network structure, its preparation method and application.
[0005] To achieve the above objectives, the present invention adopts the following technical solution:
[0006] A high-mobility-number solid electrolyte with a high-strength and high-toughness semi-interpenetrating network structure; the solid electrolyte comprises a sulfonated high ion-conductivity self-polymerizing microporous polymer (FHPIM), a linear polymer, a lithium salt, and solvent II.
[0007] The structural formula of the highly ion-conducting self-polymerizing microporous polymer (HCPIM) is shown in Formula I:
[0008] (Formula I);
[0009] In formula I, R comes from a phenolic monomer, and its structural formula is shown in any one of formula II. For connection positions;
[0010]
[0011]
[0012] (Formula II).
[0013] In Equation I, the degree of polymerization x of HCPIM ranges from 10. 2 -10 5 Between. The sites on the HCPIM that are reactively grafted are -OH sites or -COOH sites.
[0014] The high ion-conducting self-polymer microporous polymer (HCPIM) serves as the basic polymer raw material for the preparation of FHPIM, which is obtained by sulfonation of HCPIM.
[0015] Further, the weight ratio of the sulfonated high ion-conductivity self-conducting microporous polymer to the linear polymer is 1:(0.3-8), preferably 1:(1-8), and more preferably 1:(1-2.7); based on the total weight of the solid electrolyte, the total content of the sulfonated high ion-conductivity self-conducting microporous polymer and the linear polymer is 25-70 wt%, preferably 30-60 wt%, and more preferably 40-60 wt%; the content of the lithium salt is 20-60 wt%, preferably 25-50 wt%, and more preferably 25-45 wt%; the content of solvent II is 10-25 wt%, preferably 15-25 wt%, and more preferably 15-20 wt%.
[0016] Further, the linear polymer is at least one of PEO, PVDF, PVDF-HFP, PAN, and PMMA; the lithium salt includes at least one of lithium bis(trifluoromethanesulfonate)imide, lithium hexafluorophosphate, lithium bis(fluorosulfonyl)imide, lithium perchlorate, lithium tetrafluorophosphate, lithium difluorophosphate, lithium bis(oxalate-borate), and lithium di(oxalate-borate), preferably lithium bis(fluorosulfonyl)imide and / or lithium bis(trifluoromethanesulfonate); the solvent II includes at least one of tetrahydrofuran, N,N-dimethylformamide, N,N-dimethylacetamide, acetone, N-methylpyrrolidone, dimethyl sulfoxide, propylene carbonate, sulfolane, and γ-butyrolactone.
[0017] A method for preparing a high-mobility-number solid electrolyte with a high-strength, high-toughness semi-interpenetrating network structure includes the following steps:
[0018] Step 1: The high ion-conducting self-conducting microporous polymer HCPIM (shown in structural formula I), sulfonating agent, and solvent I are mixed and subjected to sulfonation reaction. After purification and drying, sulfonated high ion-conducting self-conducting microporous polymer FHPIM is obtained.
[0019] Step 2: Using the sulfonated high ion-conducting microporous polymer and the linear polymer as the basic polymer raw materials for preparing a solid electrolyte membrane with a semi-interpenetrating network structure, mix them evenly with the lithium salt and solvent II to prepare a solid electrolyte membrane solution.
[0020] Step 3: The solid electrolyte membrane solution is placed in a mold by solution casting and dried to obtain a high-mobility solid electrolyte membrane with a high-strength and high-toughness semi-interpenetrating network structure.
[0021] Furthermore, in step one, the preparation method of the highly ion-conducting self-polymerizing microporous polymer HCPIM includes the following steps:
[0022] a. Under the protection of an inert gas, pyromellitic dianhydride and methanol are reacted with catalyst 1 to generate esterification products;
[0023] b. After mixing the phenolic monomer, the esterification reaction product and solvent III, catalyst 2 is added under inert gas protection to carry out the catalytic reaction. After purification and drying, HCPIM is obtained.
[0024] Specifically,
[0025] a. Under inert gas protection, pyromellitic dianhydride and methanol are mixed uniformly at a molar ratio of 1:2, and reacted at 60-70℃ for 4-8 hours in the presence of catalyst 1 (p-toluenesulfonic acid) to generate esterification reaction product, wherein the mass of catalyst 1 (p-toluenesulfonic acid) is 3-5% of the mass of pyromellitic dianhydride;
[0026] b. One of the following phenolic monomers, such as 5,5',6,6'-tetrahydroxy-3,3,3',3'-tetramethyl-1,1'-spirobisindane, 9,10-dimethyl-9,10-ethylhexane-2,3,6,7-tetraphenol, and 9,10-dihydro-9,10-[1,2]benzo[2]benzo[2]-2,3,6,7-tetraol, the esterification reaction product, and solvent III are mixed. Under inert gas protection, potassium carbonate catalyst 2 is added to catalyze the reaction. After purification and drying, HCPIM is obtained. The molar ratio of the phenolic monomer to the esterification reaction product is 1:1. Solvent III is at least one of N,N-dimethylformamide and N-methylpyrrolidone. The mass of potassium carbonate catalyst 2 is 50-100% of the mass of the phenolic monomer. The catalytic reaction temperature is 120-150℃, and the catalytic reaction time is 24-48 h.
[0027] Furthermore, in step one, the molar ratio of the sulfonating agent to the highly ion-conducting self-polymerized microporous polymer is (0.5-2):1; the sulfonation reaction temperature is 45-60℃, and the time is 12-24h.
[0028] Furthermore, in step one, the sulfonating agent is at least one of concentrated sulfuric acid, chlorosulfonic acid, and trimethylsilylchlorosulfonate; the solvent I includes at least one of dichloromethane, chloroform, N,N-dimethylformamide, and dimethyl sulfoxide.
[0029] Furthermore, in step two, the mixing process of the sulfonated high ion-conducting microporous polymer, linear polymer, lithium salt and solvent II is carried out at a temperature of 40-60°C for 12-24 hours.
[0030] Furthermore, in step three, the drying process is vacuum drying at a temperature of 40-50℃ for 12-24 hours.
[0031] Furthermore, in step three, the prepared solid electrolyte membrane is a film with a thickness of 10-200 μm. The ion transport number of the solid electrolyte is 0.75-1.
[0032] An application of the solid electrolyte described herein or the solid electrolyte prepared by the preparation method described herein, wherein the solid electrolyte is applied to a lithium battery, the lithium battery including a lithium metal battery or a lithium-ion battery.
[0033] Compared with the prior art, the beneficial effects of the present invention are:
[0034] This invention provides a high-mobility-number solid electrolyte with a high-strength, high-toughness semi-interpenetrating network structure, its preparation method, and its applications. Through the design of a sulfonated self-polymerizing microporous polymer structure, the main molecular chain contains rigid, twisted structural units, effectively suppressing molecular chain entanglement and tight stacking. The side chains are modified with carboxylic acid and sulfonic acid functional groups (ion-conducting groups). During film formation, continuous and uniform interconnected microporous channels are formed between the polymer molecular chains. These synergistically regulate the interaction between lithium ions and solvent II, resulting in a solid electrolyte membrane with high ionic conductivity, high lithium-ion mobility, and high oxidation stability. Furthermore, the sulfonated self-polymerizing microporous polymer and the linear polymer form a unique semi-interpenetrating network structure through intermolecular synergy. This "rigid-flexible" composite system not only effectively suppresses lithium dendrite formation but also reduces interfacial impedance and improves interfacial compatibility, thereby enhancing battery cycle stability. This high-mobility-number solid electrolyte with a high-strength, high-toughness semi-interpenetrating network structure provides key material support for the development of high-safety, high-energy-density solid-state lithium batteries. Attached Figure Description
[0035] Figure 1 This is a schematic diagram of a semi-interpenetrating network structure;
[0036] Figure 2 This is a scanning electron microscope image of the solid electrolyte membrane prepared in Example 1 of the present invention;
[0037] Figure 3 This is a digital photograph of the thickness of the solid electrolyte membrane prepared in Example 1 of the present invention;
[0038] Figure 4 This is a stress-strain curve of the solid electrolyte membrane prepared in Example 1 of the present invention;
[0039] Figure 5 This is a graph showing the ionic conductivity of the solid electrolyte membrane prepared in Example 1 of the present invention.
[0040] Figure 6 The graph shows the lithium-ion transference number test results of the solid electrolyte membrane prepared in Example 1 of this invention.
[0041] Figure 7 Cyclic performance diagram of a symmetrical battery with lithium metal as both positive and negative electrodes, using the solid electrolyte membrane prepared in Example 1 of the present invention;
[0042] Figure 8 Cycle performance diagram of a battery with lithium iron phosphate as positive electrode and lithium metal as negative electrode, using the solid electrolyte membrane prepared by Example 1 and Comparative Example 1 of the present invention.
[0043] Figure 9 The diagram shows the cycle performance of a battery using the solid electrolyte membrane prepared in Example 2 of this invention, with lithium iron phosphate as the positive electrode and lithium metal as the negative electrode. Detailed Implementation
[0044] The technical solutions of the present invention will be clearly and completely described below with reference to the accompanying drawings and embodiments. Obviously, the described embodiments are only some embodiments of the invention, not all embodiments. All other embodiments obtained by those skilled in the art based on the embodiments of the present invention without creative effort are within the scope of protection of the present invention.
[0045] Example 1:
[0046] A method for preparing a high-mobility-number solid electrolyte with a high-strength, high-toughness semi-interpenetrating network structure is carried out according to the following steps:
[0047] Step 1: Preparation of highly ion-conducting self-polymerized microporous polymer.
[0048] a. Under argon protection, 21.8 g of pyromellitic dianhydride, 6.4 g of methanol, and 0.87 g of p-toluenesulfonic acid were mixed and reacted at 65 °C for 6 h. TLC was performed every 1 h during the reaction until the pyromellitic dianhydride starting material spot completely disappeared and the diester product spot appeared stably. After the reaction, the mixture was cooled to room temperature in an ice-water bath, and 40 mL of saturated NaHCO3 solution was slowly added to neutralize to pH≈7. The mixture was extracted three times with dichloromethane, and the organic phases were combined. The obtained organic phase was dried over anhydrous MgSO4, filtered, and concentrated by rotary evaporation. Subsequently, it was recrystallized with a mixed solvent (methanol:water = 4:1, volume ratio) to obtain a white crystalline esterification product.
[0049] b. 3.1 g of the esterification product and 2.86 g of 5,5',6,6'-tetrahydroxy-3,3,3',3'-tetramethyl-1,1'-spirobisindene were fully dissolved in 80 mL of anhydrous N,N-dimethylformamide solvent. 1.46 g of potassium carbonate was added as a catalyst. The mixture was stirred at 120 °C for 36 h under argon protection. After the reaction was completed, the high-viscosity reaction solution was slowly poured into pure water to obtain the crude product. The material was purified by dissolving it in chloroform and precipitating it three times from pure water. The precipitated polymer was dried overnight at 120 °C under vacuum to obtain a pale yellow high-ion-conducting self-contained microporous polymer solid, denoted as HCPIM-1.
[0050] Step 2: Preparation of sulfonated high ion-conducting self-polymerized microporous polymer.
[0051] 2g of the high ion-conducting self-conducting microporous polymer was dissolved in 40mL of anhydrous dichloromethane. Under an argon atmosphere, 3.6g of chlorosulfonic acid was slowly added dropwise (1-2 drops / second) at 50℃. The reaction was carried out for 18h, and the solution color turned light yellow. The reaction solution was cooled to 0℃ (ice-water bath), and 50mL of ice water was slowly added to quench the reaction. The precipitate was dried under vacuum at 60℃ to constant weight to obtain the sulfonated high ion-conducting self-conducting microporous polymer, denoted as FHPIM-1.
[0052] Step 3: Preparation of solid electrolyte membrane.
[0053] Under argon protection, 0.2583 g PVDF-HFP, 0.1291 g FHPIM-1 and 0.334 g LiTFSI were dissolved in a mixed solvent (THF:PC = 4:1, volume ratio) and stirred at 50 °C for 24 h to obtain a solid electrolyte membrane solution with a semi-interpenetrating network structure. The solid electrolyte membrane solution was placed in a PTFE mold and vacuum dried at 40 °C for 12 h to obtain a solid electrolyte membrane with a semi-interpenetrating network structure.
[0054] The prepared solid electrolyte membrane was scanned by electron microscopy, and the results are as follows: Figure 2 As shown, from Figure 2As can be seen from the scanning electron microscope, the solid electrolyte membrane was successfully prepared. The thickness of the prepared solid electrolyte membrane was measured, and the results are as follows... Figure 3 As shown, from Figure 3 It can be seen that the thickness of the solid electrolyte membrane is 77 μm. A thinner membrane enhances flexibility and helps optimize interfacial contact. The mechanical properties of the prepared solid electrolyte membrane were tested, and the results are as follows: Figure 4 As shown, from Figure 4 It can be seen that the elongation at break of the solid electrolyte membrane is 405%. This high elasticity allows the solid electrolyte membrane to maintain close contact during volume changes associated with lithium deposition / stripping, thus achieving dynamic interfacial adhesion. The ionic conductivity of the prepared solid electrolyte membrane was calculated using electrochemical impedance spectroscopy, and the results are as follows: Figure 5 As shown, from Figure 5 It can be seen that the solid electrolyte membrane exhibits a strength of 5.25 × 10⁻⁶ at 25 °C. -4 S cm -1 The high ionic conductivity of the prepared solid electrolyte membrane was investigated. The lithium-ion transference number was measured and calculated, and the results are as follows: Figure 6 As shown, the solid electrolyte membrane exhibits a high lithium-ion transference number of 0.76, indicating that the electrolyte improves the effective current density, reduces the risk of dendrite formation, and suppresses concentration polarization, which helps to improve the cycle stability of the battery.
[0055] Cyclic testing was performed on a symmetrical battery with lithium metal as both positive and negative electrodes (the battery used the solid electrolyte membrane prepared in Example 1 of this invention). The cyclic test results are as follows: Figure 7 As shown, the battery operates at 0.1 mA cm -2 0.1mAh cm -2 The stable cycling of more than 1000 hours under the specified conditions demonstrates the good interfacial stability of the solid electrolyte membrane prepared in Example 1 with lithium metal.
[0056] A battery using lithium iron phosphate (LFP) as the positive electrode and lithium metal as the negative electrode (this battery uses the solid electrolyte membrane prepared in Example 1 of this invention) was subjected to cycle testing, and the cycle test results are as follows: Figure 8 As shown, this battery can stably cycle for over 1000 times at a 1C rate, with a maximum discharge specific capacity of 132.2 mAh g. -1 The capacity retention rate is 80.3%, and the coulombic efficiency is above 99.96%.
[0057] Example 2:
[0058] A method for preparing a high-mobility-number solid electrolyte with a high-strength, high-toughness semi-interpenetrating network structure is carried out according to the following steps:
[0059] Step 1: Preparation of highly ion-conducting self-polymerized microporous polymer.
[0060] a. The esterification product was prepared using the same method as in Example 1;
[0061] b. Dissolve 2.18 g of the esterification product and 3.01 g of 9,10-dimethyl-9,10-ethylhexane-2,3,6,7-tetraphenol in 80 mL of anhydrous DMF solvent, add 2.41 g of potassium carbonate as a catalyst, and stir at 135 °C for 36 h under argon protection. After the reaction is completed, slowly pour the high-viscosity reaction solution into pure water to obtain the crude product. Purify the material by dissolving it in DMF and precipitating it from pure water three times. Freeze-dry the precipitated polymer at -50 °C for 48 h to obtain a dark brown high ion-conducting self-contained microporous polymer solid, denoted as HCPIM-2.
[0062] Step 2: Preparation of sulfonated high ion-conducting self-polymerized microporous polymer.
[0063] 2g of the high ion-conducting self-conducting microporous polymer was dissolved in 40mL of DMSO solvent. Under an argon atmosphere and in an ice-water bath (0-10℃), 4g of trimethylsilylchlorosulfonate was slowly added dropwise (completed within 30min). The temperature was then raised to 50℃ and the reaction was allowed to proceed for 20h. The reaction solution was cooled to 0℃ (ice-water bath), and 10mL of methanol was slowly added to quench the reaction. The mixture was washed three times with diethyl ether and pure water, and the precipitate was dried under vacuum at 60℃ to constant weight to obtain the sulfonated high ion-conducting self-conducting microporous polymer, denoted as FHPIM-2.
[0064] Step 3: Preparation of solid electrolyte membrane.
[0065] Under argon protection, 0.129 g PVDF-HFP, 0.129 g FHPIM-2 and 0.155 g LiTFSI were dissolved in a mixed solvent (THF:NMP = 3:1, volume ratio) and stirred at 50 °C for 24 h to obtain a solid electrolyte membrane solution with a semi-interpenetrating network structure. The solid electrolyte membrane solution was placed in a PTFE mold and vacuum dried at 40 °C for 12 h to obtain a solid electrolyte membrane with a semi-interpenetrating network structure and a thickness of 65 μm.
[0066] A battery using lithium iron phosphate (LFP) as the positive electrode and lithium metal as the negative electrode (this battery uses the solid electrolyte membrane prepared in Example 2 of this invention) was subjected to cycle testing, and the cycle test results are as follows: Figure 9 As shown, this battery can stably cycle for over 1000 cycles at a 1C rate, with a maximum discharge specific capacity of 134.84 mAh g. -1 The capacity retention rate was 83.7%, and the coulomb efficiency exceeded 99.99%.
[0067] Comparative Example 1:
[0068] Under argon protection, 0.258 g of PVDF-HFP was added to 8 mL of THF solvent and stirred at 40 °C for 24 h to form a homogeneous polymer solution. Simultaneously, 0.334 g of LiTFSI was dissolved in 4 mL of DMSO and stirred at room temperature for 24 h to form a salt solution. The two solutions were mixed and stirred at room temperature for 24 h to obtain a solid electrolyte membrane solution. The solid electrolyte membrane solution was placed in a PTFE mold and vacuum dried at 40 °C for 12 h to obtain a solid electrolyte membrane with a thickness of 98 μm.
[0069] A battery using lithium iron phosphate (LFP) as the positive electrode and lithium metal as the negative electrode (this battery uses the solid electrolyte membrane prepared in Comparative Example 1 of this invention) was subjected to cycle testing, and the cycle test results are as follows: Figure 8 As shown, the battery achieves a maximum discharge specific capacity of 152.3 mAh g at a 1C rate. -1 After 360 cycles, the capacity decreased to 104.06 mAh g. -1 The capacity retention rate was 68.3%.
[0070] Table 1 Performance data of each embodiment and comparative example
[0071]
[0072] Table 1 shows the room temperature conductivity and lithium-ion transference number of the solid electrolyte membranes that can be prepared. Any solid electrolyte materials not listed in Table 1 that are prepared by simply modifying the method described in this invention are still within the scope of this invention.
[0073] The high-mobility-number solid electrolyte with a high-strength and high-toughness semi-interpenetrating network structure proposed in this invention is composed of a functionalized high-ionic-conductivity self-polymerizing microporous polymer (FHPIM) and a linear polymer. FHPIM is a functional material prepared by grafting ester monomers with aromatic rings and then sulfonating them. Its molecular structure, with uniformly distributed sulfonic acid groups (-SO3H) and carboxylic acid groups (-COOH) and continuously interconnected microporous channels, jointly constructs a highly efficient lithium-ion transport network, enabling the electrolyte to possess both high ionic conductivity and high lithium-ion mobility. The rigid framework of the sulfonated self-polymerizing microporous polymer material and the flexible segments of the linear polymer synergistically form a semi-interpenetrating network structure that combines rigidity and flexibility. This structure can restrict anion transport and provide interconnected ion channels with continuous micropores and uniform pore distribution for lithium-ion transport, further improving ionic conductivity. It significantly outperforms traditional linear polymer electrolyte systems in terms of cycle stability and interfacial kinetics. The solid electrolyte provided by this invention has superior overall performance, effectively solving the technical problem of balancing mechanical strength and ionic conductivity in existing polymer electrolytes, and providing key material support for the development of high-safety, high-energy-density solid-state lithium batteries.
[0074] Furthermore, it should be understood that although this specification describes embodiments, not every embodiment contains only one independent technical solution. This narrative style is merely for clarity. Those skilled in the art should consider the specification as a whole, and the technical solutions in each embodiment can also be appropriately combined to form other embodiments that can be understood by those skilled in the art.
Claims
1. A high-mobility solid-state electrolyte with a high-strength high-toughness semi-interpenetrating network structure, characterized by: The solid-state electrolyte has a high-strength and high-toughness semi-interpenetrating network structure; the solid-state electrolyte comprises a sulfonated high-ionic-conducting self-polymer microporous polymer, a linear polymer, a lithium salt and a solvent II. 2.The high-mobility solid-state electrolyte with high-strength and high-toughness semi-interpenetrating network structure according to claim 1, characterized in that: The high-ionic-conducting self-polymer microporous polymer has a structural formula as shown in Formula I: Formula I; wherein the structure of R in Formula I is represented by any one of Formula II, and is a linking position; Formula II.
3. The high-mobility solid-state electrolyte with high-strength and high-toughness semi-interpenetrating network structure according to claim 2, characterized in that: The value of the polymerization degree x in the formula I is in the range of 10 2 -10 5 .
4. The high-mobility solid-state electrolyte with high-strength and high-toughness semi-interpenetrating network structure according to claim 1, characterized in that: The weight ratio of the sulfonated high-ionic-conducting self-polymer microporous polymer to the linear polymer is 1:(0.3-8); in the solid-state electrolyte, the total content of the sulfonated high-ionic-conducting self-polymer microporous polymer and the linear polymer accounts for 25-70 wt%, the content of the lithium salt accounts for 20-60 wt%, and the content of the solvent II accounts for 10-25 wt%.
5. The high-mobility solid-state electrolyte with high-strength and high-toughness semi-interpenetrating network structure according to claim 1, characterized in that: The linear polymer is at least one of PEO, PVDF, PVDF-HFP, PAN and PMMA; the lithium salt comprises at least one of lithium bis(trifluoromethanesulfonyl)imide, lithium hexafluorophosphate, lithium bis(fluorosulfonyl)imide, lithium perchlorate, lithium tetrafluorophosphate, lithium difluorophosphate, lithium bis(oxalato)borate and lithium difluoro(oxalato)borate; the solvent II comprises at least one of tetrahydrofuran, N,N-dimethylformamide, N,N-dimethylacetamide, acetone, N-methylpyrrolidone, dimethyl sulfoxide, propylene carbonate, sulfolane and gamma-butyrolactone.
6. A method for preparing the high-mobility solid-state electrolyte with high-strength and high-toughness semi-interpenetrating network structure according to any one of claims 2-5, characterized in that, The method comprises the following steps: Step one, the high-ionic-conducting self-polymer microporous polymer shown in Formula I, a sulfonating agent and a solvent I are mixed to undergo a sulfonation reaction, and then are purified and dried to obtain the sulfonated high-ionic-conducting self-polymer microporous polymer; Step two, the sulfonated high-ionic-conducting self-polymer microporous polymer and the linear polymer are used as basic polymer raw materials, and are mixed with the lithium salt and the solvent II to obtain a solid-state electrolyte film liquid; Step three, the solid-state electrolyte film liquid is placed in a mold by a solution casting method and is dried to obtain a high-mobility solid-state electrolyte film having a high-strength and high-toughness semi-interpenetrating network structure.
7. The method of claim 6, wherein: In step one, the molar ratio of the sulfonating agent to the high-ionic-conducting self-polymer microporous polymer is (0.5-2):1; the sulfonation reaction is performed at a temperature of 45-60°C for 12-24 hours.
8. The method of claim 6, wherein: In step one, the sulfonating agent is at least one of concentrated sulfuric acid, chlorosulfonic acid and trimethylsilyl chlorosulfate; and the solvent I comprises at least one of dichloromethane, chloroform, N,N-dimethylformamide and dimethyl sulfoxide.
9. The method of claim 6, wherein: In step three, the prepared solid-state electrolyte film has a thickness of 10-200 μm.
10. Use of a solid state electrolyte according to any one of claims 1 to 5 or a solid state electrolyte produced by the method according to any one of claims 6 to 9, characterized in that: The solid-state electrolyte is applied to a lithium battery.