Micro-phase separation high-pressure-resistant high-elasticity solid-state electrolyte and preparation and application thereof

Abstract

The application discloses a kind of micro phase separation high-pressure resistant high elasticity solid electrolyte and its preparation and application, it is related to lithium battery technical field.The raw material of the present application includes fluorine-containing acrylate structure inducing monomer containing >=C8 fluorine alkyl side chain, amorphous short side chain acrylate / acrylamide type adjusting monomer, lithium salt and ion liquid / deep eutectic composition of ion conducting phase, which is prepared by mixing copolymerization to obtain the solid electrolyte.The application builds the system of ordered micro phase separation structure, functional partition matching and ion efficient transmission through the molecular synergistic effect between components, and further breaks through the technical bottleneck of traditional polymer-based solid electrolyte in mechanical property, high-pressure stability and ion conduction efficiency, realizes the optimization of electrolyte performance from the microstructure design level, and provides a feasible path for the industrialization of solid-state lithium battery.

Description

Technical Field

[0001] This invention relates to the field of lithium battery technology, and in particular to a microphase-separated, high-voltage-resistant, high-elasticity solid electrolyte and its preparation and application. Background Technology

[0002] With the rapid development of high-power electronics and new energy fields such as 5G communication, portable energy storage devices and electric vehicles, end products have placed higher demands on the performance of lithium-ion batteries. They not only need to have high energy density to meet the demand for long driving range, but also need to take into account excellent safety to avoid risks such as thermal runaway. The synergistic improvement of both has become the core goal of industry research and development.

[0003] Among numerous battery technologies, solid-state lithium batteries, which use solid electrolytes instead of traditional liquid electrolytes and possess both intrinsic flame retardancy and high energy density potential, are considered an important development direction for overcoming existing technological bottlenecks. Polymer-based solid electrolytes, in particular, have shown significant potential in the industrialization of solid-state lithium batteries due to their convenient processing, relatively low production costs, and good compatibility with electrode interfaces, making them one of the key research areas currently.

[0004] However, traditional polymer-based solid electrolytes still generally face the following technical bottlenecks, which seriously restrict their practical application: (1) Insufficient mechanical strength and toughness. Most polymer matrices are flexible chain structures. The electrolyte film formed after curing has weak tensile and puncture resistance, making it difficult to effectively suppress the growth of lithium dendrites on the surface of the lithium metal anode during the charging and discharging process of lithium batteries. The continuous growth of lithium dendrites can easily puncture the electrolyte film, causing short circuits between the positive and negative electrodes, which directly threatens battery safety. (2) Narrow electrochemical stability window, making it difficult to match the stable cycling of high-voltage positive electrodes. (3) Low room temperature ionic conductivity. The polymer molecular chains have weak mobility at room temperature, and the migration path of lithium ions in them is discontinuous. The conductivity is much lower than that of liquid electrolytes, which limits the rate performance and low-temperature performance of the battery.

[0005] To overcome these bottlenecks, existing research often prioritizes enhancing mechanical properties, such as increasing the degree of polymer crosslinking to construct a denser network structure or introducing inorganic rigid particles as reinforcing phases. However, such methods often face the challenge of performance trade-offs. Excessive crosslinking can restrict the movement of polymer molecular chains and block lithium-ion conduction channels; while the introduction of rigid particles, if unevenly dispersed, can easily form interface defects, similarly disrupting the continuity of ion conduction. Ultimately, it is difficult to achieve synergistic optimization of mechanical support, ion conduction, and high-pressure stability.

[0006] Simply adjusting macroscopic components or optimizing a single performance aspect is no longer sufficient to meet the comprehensive performance requirements of solid-state lithium batteries for electrolytes. The industry urgently needs a new synergistic regulation strategy that starts from molecular design and microstructure. By constructing an electrolyte structure that combines ordered functional partitions with a continuous conduction network, issues such as mechanical strength, ionic conductivity, and high-voltage stability can be addressed, providing key technological support for performance breakthroughs and industrial applications of solid-state lithium batteries. Summary of the Invention

[0007] The purpose of this invention is to provide a microphase-separated, high-pressure-resistant, and highly elastic solid electrolyte, as well as its preparation and application, to solve the problems existing in the prior art.

[0008] To achieve the above objectives, the present invention provides the following solution: This invention provides a microphase-separated, high-pressure-resistant, and highly elastic solid electrolyte, the raw material components of which include: Structure-induced monomers, shape-modulating monomers, and ion-conducting phases; The molar percentage of the ion-conducting phase is 40-60 mol, the molar percentage of the inducing monomer is 2.5-20 mol, and the molar percentage of the shaping monomer is 20-55 mol%. The structure-inducing monomer is a fluorinated acrylate monomer containing a ≥C8 fluoroalkyl side chain; The shape-modulating monomers are amorphous, rubbery acrylate monomers or acrylamide monomers; they are used to regulate morphology and suppress excessive ordering, as well as to enhance the competitiveness of molecular interactions. The acrylate monomers have ≤4 carbon atoms in their side chains and are not 0; the acrylamide monomers have ≤4 carbon atoms in their side chains and are not 0. The ion-conducting phase is a mixture of lithium salt and ionic liquid or a mixture of lithium salt and deep eutectic.

[0009] When the ion-conducting phase is a mixture of lithium salt and ionic liquid, the lithium salt is 50-80 mol% of the ionic liquid. When the ion-conducting phase is a mixture of lithium salt and deep eutectic, the molar percentage of the lithium salt is 10-20 mol.

[0010] Furthermore, the structure-inducing monomer is perfluorooctyl ethyl acrylate.

[0011] Furthermore, the acrylate monomers may be selected from, but are not limited to, at least one of butyl acrylate, polyethylene glycol monomethyl ether methacrylate, and ethyl acrylate; the acrylamide monomers may be selected from, but are not limited to, N,N-dimethylacrylamide.

[0012] Furthermore, the lithium salt is selected from at least one of lithium bis(trifluoromethanesulfonyl)imide, lithium bis(fluorosulfonyl)imide, and lithium difluorooxalateborate; the ionic liquid is selected from at least one of imidazole-type ionic liquids and pyrrolidineonium-type ionic liquids.

[0013] Furthermore, the deep eutectic is formed by mixing an amide solvent with a lithium salt in a molar ratio of 5:1; the amide solvent is N-methyl-2,2,2-trifluoroacetamide or N-methylacetamide.

[0014] Further, the imidazole-type ionic liquid is 1-butyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide salt; the pyrrolidine-onium-type ionic liquid is 1-n-butyl-1-methylpyrrolidine bis(trifluoromethanesulfonyl)imide.

[0015] Furthermore, the raw material components also include crosslinking agents and photoinitiators.

[0016] The crosslinking agent includes polyethylene glycol diacrylate, and the photoinitiator includes photoinitiator 184.

[0017] The fluorinated side-chain structure-induced monomer provides a key foundation for the structural design of the solid electrolyte of this invention: when the length of the fluorinated side-chain group reaches a threshold (e.g., ≥C8), its chemical incompatibility with the hydrocarbon backbone (or matrix) is significantly enhanced, leading to the spontaneous formation of a microphase separation structure. This self-organizing behavior further enables clear functional partitioning, with the elastic continuous phase providing mechanical support and deformation buffering, while the fluorine-rich phase enhances the stability and oxidation resistance of the electrode interface. Simultaneously, by controlling the morphology and orientation of the microphase, continuous conduction channels can be reserved for the ion-conducting phase.

[0018] To avoid problems such as embrittlement and ion channel blockage caused by excessive crystallization or orientation of the matrix, copolymerizing long-fluorinated side-chain monomers with amorphous, rubbery short-side-chain acrylates or short-side-chain acrylamide monomers can yield a matrix with good flexibility and tunable morphology. Introducing ionic liquids as the ion-conducting phase further enables the construction of a continuous and stable ion transport network within the microphase-separated framework, ultimately effectively improving the room-temperature ionic conductivity while ensuring the electrolyte's elasticity and structural stability.

[0019] The present invention also provides a method for preparing the above-mentioned microphase-separated high-pressure resistant and high-elasticity solid electrolyte, comprising the following steps: mixing raw material components and copolymerizing to obtain the microphase-separated high-pressure resistant and high-elasticity solid electrolyte.

[0020] The copolymerization methods include solution polymerization, in-situ polymerization, or photo / thermal curing, thereby achieving network formation and inducing the formation of a microphase separation structure consisting of a fluorine-rich phase and an elastic continuous phase.

[0021] Furthermore, the present invention can introduce an ion-conducting phase during the polymerization process or post-processing, and control the microphase morphology and orientation through the ratio, curing conditions and post-processing to achieve the continuity and stability of the ion-conducting channels.

[0022] The microphase structure of the present invention is preferably arranged in a layered or quasi-layered orientation to balance mechanical support and ion channel continuity.

[0023] This invention can achieve the integrated construction of electrolyte film and electrode interface by in-situ polymerization or photo / thermal curing process.

[0024] The present invention further provides the application of the above-mentioned microphase-separated high-voltage-resistant and high-elasticity solid electrolyte in lithium-ion batteries.

[0025] Furthermore, the solid electrolyte of the present invention can be used as an electrolyte in lithium nickel cobalt manganese oxide (NCM811) cathodes.

[0026] Furthermore, NCM811 can be used as the active material, Super P as the conductive additive, polyvinylidene fluoride as the binder, and N-methylpyrrolidone as the solvent. An electrolyte is also added, and the components are thoroughly mixed and stirred until the system is homogeneous to prepare the positive electrode slurry. This slurry is then uniformly coated onto the surface of aluminum foil, dried to remove the solvent, and cut into electrode sheets of a specified size to obtain the NCM811 positive electrode. After the positive electrode preparation is complete, the NCM811 positive electrode is used as the positive electrode sheet, combined with the aforementioned prepared solid electrolyte and lithium foil (as the negative electrode), and assembled sequentially according to conventional lithium battery assembly processes to form a lithium battery.

[0027] This invention constructs an ordered microphase separation structure, functional partition matching, and efficient ion transport system through molecular synergistic effects between components, thereby breaking through the technical bottlenecks of traditional polymer-based solid electrolytes in terms of mechanical properties, high-pressure stability, and ion conduction efficiency, and optimizing electrolyte performance from the microstructure design level.

[0028] The spontaneous formation of the microphase separation structure in this invention is the basis for performance optimization. The ≥C8 fluoroalkyl side chains of structure-induced monomers (such as the long fluoro side chains of perfluorooctyl ethyl acrylate) exhibit significant chemical incompatibility with the hydrocarbon segments of shape-modifying monomers (amorphous, rubbery short-chain acrylates or acrylamides). This difference in intermolecular interfacial energy drives the system to spontaneously separate during polymerization, forming two functionally distinct microphases: one is an elastic continuous phase dominated by shape-modifying monomers, whose rubbery properties provide sufficient flexibility and mechanical buffering capacity, which can adapt to the volume deformation during battery charging and discharging, and can also physically block the growth and puncture of lithium dendrites on the surface of lithium metal anodes with good toughness, solving the problem of insufficient mechanical strength of traditional electrolytes; the other is a fluorine-rich microphase with ordered stacking of fluorine side chains of structure-induced monomers. The high electronegativity and chemical inertness of fluorine enable it to form a stable interfacial layer at the electrolyte-electrode interface, which can suppress the oxidative decomposition of electrode materials and electrolyte side reactions, and broaden the electrochemical stability window, allowing the electrolyte to be adapted to high-voltage cathode materials and achieve high-voltage resistance.

[0029] The synergistic effect of the structural characteristics of the shape-modulating monomer and the ion-conducting phase in this invention ensures efficient ion transport. The amorphous structure of the shape-modulating monomer avoids matrix embrittlement caused by excessive crystallization or excessive orientation of fluorine side chains. Simultaneously, its short side chain structure does not block the continuous channels reserved for microphase separation, providing ample space for the filling and migration of the ion-conducting phase. In the ion-conducting phase, the lithium salt, acting as a lithium-ion source, forms a stable lithium-ion solvation sheath under the solvation action of ionic liquids or deep eutectic. Utilizing the liquid properties of ionic liquids / deep eutectic, it fully fills the continuous channels formed by microphase separation, ultimately constructing an ion transport network that runs throughout the entire electrolyte. Lithium ions can migrate smoothly along this network, significantly improving room-temperature ionic conductivity and lithium-ion transference number, thus solving the problem of low room-temperature ion conduction efficiency in traditional polymer electrolytes.

[0030] This invention utilizes the solid electrolyte in lithium-ion batteries, simultaneously optimizing mechanical dendrite suppression, high-voltage stability, and high room-temperature conductivity within the same material system: the elastic continuous phase provides load-bearing and buffering capabilities, significantly improving crack and puncture resistance while suppressing lithium dendrite penetration; the fluorine-rich phase enhances oxidation stability and interfacial compatibility, adapting to stable cycling at high voltages (3.0-4.5V voltage window); and the continuous ion-conducting network within the microphase framework ensures a room-temperature ionic conductivity ≥1×10⁻⁶. - 4 S·cm -1 Through controllable microphase separation and morphology adjustment, a comprehensive balance can be further achieved in terms of mechanics, conductivity, and high-pressure stability.

[0031] This invention achieves functional complementarity by inducing microphase separation through molecular design and microphase partitioning, and constructing a continuous transport network through ion-conducting phases. It can achieve synergistic optimization of mechanical dendrite suppression, high-voltage stability and high room-temperature conductivity within the same material system, and ultimately optimize the performance of electrolyte with high elastic mechanical support, high-voltage interface stability and high room-temperature ion conduction, precisely matching the electrolyte performance requirements of solid-state lithium batteries.

[0032] The present invention discloses the following technical effects: This invention achieves technological innovation by inducing microphase separation through molecular design, synergistic functional partitioning, and ion network construction, addressing the technical problems of traditional polymer-based solid electrolytes. It demonstrates significant advantages in mechanical safety, ion conduction, high-voltage adaptability, and industrial applications. (1) Improved mechanical properties: This invention utilizes the chemical incompatibility between long fluorine side chains and hydrocarbon segments to construct a microphase separation structure. The elastic continuous phase, mainly composed of shape-modulating monomers, has excellent flexibility and toughness, with an elongation at break of up to 452%. This not only adapts to the volume deformation of the electrodes during the charging and discharging of lithium batteries, avoiding electrolyte rupture caused by stress concentration, but also inhibits the growth and puncture of lithium dendrites on the surface of lithium metal anodes through physical barrier effects, thereby reducing the risk of short circuits between positive and negative electrodes from the root and solving the technical problem that the insufficient mechanical strength of traditional electrolytes easily leads to safety hazards.

[0033] (2) Room temperature ion conductivity meets practical requirements: This invention reserves continuous channels by shaping the amorphous structure of the monomer, and with the filling of ionic liquid / deep eutectic ion-conducting phase, an ion transport network is constructed throughout the electrolyte, which effectively solves the problems of weak molecular chain motion and discontinuous ion conduction paths in traditional polymer electrolytes at room temperature. The room temperature ion conductivity of the electrolyte can reach 6.8 × 10⁻⁶. -4 S·cm -1 The lithium-ion transference number has been increased to 0.55, which can ensure the efficient migration of lithium ions at room temperature to meet the battery's rate discharge performance requirements, and can also be adapted to low-temperature working scenarios, breaking the technical limitation of traditional polymer electrolytes that can only achieve high conductivity at high temperatures.

[0034] (3) Optimization of high voltage stability and electrode compatibility: The fluorine-rich microphase in the microphase separation structure can form a stable protective layer at the interface between the electrolyte and the electrode (especially the high voltage positive electrode) due to the high electronegativity and chemical inertness of fluorine. On the one hand, it inhibits the oxidation and decomposition of the positive electrode material and the side reaction of the electrolyte under high voltage. On the other hand, it broadens the electrochemical stability window of the electrolyte to above 4.5V, effectively solving the problem that the traditional electrolyte has a narrow electrochemical stability window and cannot be adapted to the high voltage positive electrode, providing key support for improving the energy density of lithium batteries.

[0035] This invention employs a preparation route involving room temperature stirring and ultraviolet light curing. The process steps are simple and controllable, requiring no complex conditions such as high temperature and high pressure. Furthermore, the raw material components are all conventionally available chemicals that can be mass-produced, which reduces production energy consumption and costs while ensuring batch stability of the product. At the same time, the electrolyte obtained is a self-supporting film that can be directly adapted to the existing lithium battery stacking and assembly process without requiring significant modifications to the production line, thus providing a feasible path for the industrialization of solid-state lithium batteries. Attached Figure Description

[0036] To more clearly illustrate the technical solutions in the embodiments of the present invention or the prior art, the drawings used in the embodiments will be briefly introduced below. Obviously, the drawings described below are only some embodiments of the present invention. For those skilled in the art, other drawings can be obtained based on these drawings without creative effort.

[0037] Figure 1 The stress-strain curve of the solid electrolyte material prepared in Example 1 of this invention is shown.

[0038] Figure 2 Optical photographs of solid electrolyte materials with different perfluorooctyl ethyl acrylate contents in Example 1 of this invention.

[0039] Figure 3 The image shows SEM images of solid electrolyte materials with different perfluorooctyl ethyl acrylate contents in Example 1 of this invention.

[0040] Figure 4 The impedance spectra of the solid electrolyte material prepared in Example 1 of this invention at different temperatures are shown.

[0041] Figure 5 The lithium-ion transference number at room temperature is the solid electrolyte material prepared in Example 1 of this invention.

[0042] Figure 6 The graph shows the cycling performance of the NCM811 / Li lithium battery prepared based on the solid electrolyte material of Example 1 of this invention in a wide electrochemical window of 3.0-4.5. Detailed Implementation

[0043] Various exemplary embodiments of the present invention will now be described in detail. This detailed description should not be considered as a limitation of the present invention, but rather as a more detailed description of certain aspects, features, and embodiments of the present invention.

[0044] It should be understood that the terminology used in this invention is merely for describing particular embodiments and is not intended to limit the invention. Furthermore, with respect to numerical ranges in this invention, it should be understood that each intermediate value between the upper and lower limits of the range is also specifically disclosed. Any stated value or intermediate value within a stated range, as well as each smaller range between any other stated value or intermediate value within said range, is also included in this invention. The upper and lower limits of these smaller ranges may be independently included or excluded from the range.

[0045] Unless otherwise stated, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art. While only preferred methods and materials have been described herein, any methods and materials similar or equivalent to those described herein may be used in the implementation or testing of this invention. All references to this specification are incorporated by way of citation to disclose and describe methods and / or materials associated with those references. In the event of any conflict with any incorporated reference, the content of this specification shall prevail.

[0046] Various modifications and variations can be made to the specific embodiments described in this specification without departing from the scope or spirit of the invention, as will be apparent to those skilled in the art. Other embodiments derived from this specification will also be readily apparent to those skilled in the art. This specification and embodiments are merely exemplary.

[0047] The terms “include,” “including,” “have,” “contain,” etc., used in this article are all open-ended terms, meaning that they include but are not limited to.

[0048] It should be noted that any aspects not described in detail in this invention are conventional practices in the field and are not the focus of this invention.

[0049] Example 1 This embodiment provides a microphase-separated solid elastic electrolyte, the steps of which are as follows: Prepare the raw materials according to the following dosages: Perfluorooctyl ethyl acrylate (1 mmol) is used as the structure-inducing monomer; ethyl acrylate (9 mmol) is used as the shape-modifying monomer; the ion-conducting phase consists of a lithium salt and an ionic liquid, wherein the lithium salt is lithium bis(trifluoromethanesulfonyl)imide (6.5 mmol, corresponding to 65 mol% of the ionic liquid), and the ionic liquid is 1-n-butyl-1-methylpyrrolidine di(trifluoromethanesulfonyl)imide (10 mmol); a crosslinking agent and a photoinitiator are also used, the crosslinking agent is polyethylene glycol diacrylate (number average molecular weight Mw = 200, 0.5 mol% of the total system weight), and the photoinitiator is photoinitiator 184 (0.1 mol% of the total system weight).

[0050] All the above raw materials were added to the reaction vessel in sequence and stirred at a constant speed for 30 min at room temperature until a uniform, transparent prepolymer liquid without obvious particles or stratification was formed. After polymerization by ultraviolet light irradiation (365nm ultraviolet irradiation for 1 h), a self-supporting highly elastic solid electrolyte was obtained.

[0051] The prepared solid electrolyte material was subjected to performance tests. The results showed that its tensile strength at break was 0.38 MPa and its elongation at break was 452%, exhibiting excellent elasticity and toughness. It can effectively cope with volume deformation and mechanical impact during battery charging and discharging. The specific stress-strain curve is shown in Figure 1. Furthermore, optical microscopy revealed that with the increase of perfluorooctyl ethyl acrylate content (the molar content of perfluorooctyl ethyl acrylate varied from 0-15 mol%), the microphase separation phenomenon caused by the incompatibility of fluorine and hydrocarbon components within the electrolyte gradually became more significant. The system gradually transformed from a homogeneous and transparent state to a state with a clear phase region structure, which directly confirmed the inducing effect of long fluorine side chains on the microphase separation structure. The specific appearance and phase region changes are shown in Figure 2 and Figure 3. Figure 3 As shown.

[0052] The room temperature ion conductivity of the electrolyte was tested. Figure 4 Impedance spectra of the solid electrolyte material prepared in Example 1 of this invention at different temperatures; Figure 5 The value represents the lithium-ion transference number at room temperature of the solid electrolyte material prepared in Example 1 of this invention. The results show that its room-temperature ionic conductivity can reach 6.8 × 10⁻⁶. -4 S·cm -1 The lithium-ion transference number is 0.55, indicating that the elastic electrolyte has excellent room-temperature ion transport capability and can meet the performance requirements of lithium batteries for ion conduction efficiency.

[0053] Using the prepared elastic solid electrolyte as the ion-conducting medium, and combining it with NCM811 cathode material and lithium foil anode, a pouch lithium battery was assembled. The electrochemical performance of this lithium battery was tested, and the results showed that it could achieve stable cycling within a high voltage window of 4.5V. During cycling, the capacity decay was gradual and the voltage plateau was stable. Specific cycling performance curves are shown below. Figure 6 As shown, this elastic solid electrolyte possesses excellent high-voltage tolerance and electrode interface compatibility, enabling it to meet the requirements of high-voltage cathode materials and providing support for improving the energy density of lithium batteries.

[0054] Example 2 This embodiment provides a microphase-separated solid elastic electrolyte, the steps of which are as follows: Prepare the raw materials according to the following dosages: the structure-inducing monomer is perfluorooctyl ethyl acrylate (1 mmol), the shape-modifying monomer is polyethylene glycol monomethyl ether methacrylate (9 mmol), the ion-conducting phase consists of lithium salt and ionic liquid (lithium salt is lithium bis(trifluoromethanesulfonyl)imide (6.5 mmol, the lithium salt content corresponds to 65 mol% of the ionic liquid); the ionic liquid is 1-butyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide (10 mmol), and the crosslinking agent polyethylene glycol diacrylate (number average molecular weight Mw=200, the dosage is 0.5 mol% of the total system) and photoinitiator 184 (the dosage is 0.1 mol% of the total system) are used.

[0055] Example 3 This embodiment provides a microphase-separated elastic solid electrolyte, the steps of which are as follows: Prepare the raw materials according to the following dosages: the structure-inducing monomer is perfluorooctyl ethyl acrylate (1 mmol), the shape-modifying monomer is polyethylene glycol monomethyl ether methacrylate (9 mmol), the ion-conducting phase is a deep eutectic with a specific ratio (10 mmol, which is prepared by mixing N-methyl-2,2,2-trifluoroacetamide and lithium difluorooxalate borate in a molar ratio of 5:1), and the crosslinking agent polyethylene glycol diacrylate (number average molecular weight Mw=200, amount of which is 0.5 mol% of the total system) and photoinitiator 184 (amount of which is 0.1 mol% of the total system) are used.

[0056] Example 4 This embodiment provides a microphase-separated elastic solid electrolyte, the steps of which are as follows: Prepare the raw materials according to the following dosages: the structure-inducing monomer is perfluorooctyl ethyl acrylate (1 mmol); the shape-modifying monomer is N,N-dimethylacrylamide (9 mmol); the ion-conducting phase is a custom-formulated deep eutectic (10 mmol, which is prepared by mixing N-methyl-2,2,2-trifluoroacetamide and lithium bis(trifluoromethanesulfonyl)imide in a molar ratio of 5:1); and the crosslinking agent polyethylene glycol diacrylate (number-average molecular weight Mw=200, amounted to 0.5 mol% of the total system) and photoinitiator 184 (amounted to 0.1 mol% of the total system) are used.

[0057] Example 5 This embodiment provides a microphase-separated elastic solid electrolyte, the steps of which are as follows: Prepare the raw materials according to the following dosages: the structure-inducing monomer is perfluorooctyl ethyl acrylate (1 mmol), the shape-modifying monomer is butyl acrylate (9 mmol), and the ion-conducting phase consists of lithium salt and ionic liquid (lithium bis(trifluoromethanesulfonyl)imide, 6.5 mmol; ionic liquid is 1-butyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide, 10 mmol). At the same time, use polyethylene glycol diacrylate (number average molecular weight Mw=200, 0.5 mol% of the total system) as a crosslinking agent and photoinitiator 184 (0.1 mol% of the total system).

[0058] The solid electrolytes prepared in Examples 2-5 were subjected to the same performance tests as in Example 1, and the results are shown in Table 1: Table 1 The embodiments described above are merely preferred embodiments of the present invention and are not intended to limit the scope of the present invention. Various modifications and improvements made by those skilled in the art to the technical solutions of the present invention without departing from the spirit of the present invention should fall within the protection scope defined by the claims of the present invention.

Claims

1. A microphase-separated, high-pressure-resistant, high-elasticity solid electrolyte, characterized in that, The raw material components include: Structure-inducing monomers, shape-modulating monomers, ion-conducting phases, crosslinking agents, and photoinitiators; The molar percentage of the ion-conducting phase is 40-60 mol, the molar percentage of the structure-inducing monomer is 2.5-20 mol, and the molar percentage of the shape-modulating monomer is 20-55 mol%. The structure-inducing monomer is perfluorooctyl ethyl acrylate; The shaping monomer is at least one of polyethylene glycol monomethyl ether methacrylate and ethyl acrylate, or N,N-dimethylacrylamide; The ion-conducting phase is a mixture of lithium salt and ionic liquid or a mixture of lithium salt and deep eutectic. When the ion-conducting phase is a mixture of lithium salt and ionic liquid, the lithium salt is 50-80 mol% of the ionic liquid. When the ion-conducting phase is a mixture of lithium salt and deep eutectic, the molar percentage of the lithium salt is 10-20 mol%. The deep eutectic is formed by mixing N-methyl-2,2,2-trifluoroacetamide and lithium difluorooxalate borate in a molar ratio of 5:1; or by mixing N-methyl-2,2,2-trifluoroacetamide and lithium bis(trifluoromethanesulfonyl)imide in a molar ratio of 5:

1.

2. The microphase-separated, high-pressure-resistant, high-elasticity solid electrolyte according to claim 1, characterized in that, The lithium salt is selected from at least one of lithium bis(trifluoromethanesulfonyl)imide, lithium bis(fluorosulfonyl)imide, and lithium difluorooxalateborate; the ionic liquid is selected from at least one of imidazole-type ionic liquid and pyrrolidineonium-type ionic liquid.

3. The microphase-separated, high-pressure-resistant, high-elasticity solid electrolyte according to claim 2, characterized in that, The imidazole-type ionic liquid is 1-butyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide salt; the pyrrolidine-onium-type ionic liquid is 1-n-butyl-1-methylpyrrolidine bis(trifluoromethanesulfonyl)imide.

4. The method for preparing the microphase-separated, high-pressure-resistant, and highly elastic solid electrolyte according to any one of claims 1-3, characterized in that, Includes the following steps: The raw material components are mixed and copolymerized to obtain the microphase-separated, high-pressure-resistant, and highly elastic solid electrolyte.

5. The application of the microphase-separated, high-voltage-resistant, and highly elastic solid electrolyte as described in any one of claims 1-3 in lithium-ion batteries.

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