Polymers and their use

Abstract

This application provides a polymer and its use. The polymer comprises a first block shown in Formula 1 and a second block shown in Formula 2, where R1 is selected from substituted or unsubstituted C1-C30 alkyl groups, substituted or unsubstituted polyethers, substituted or unsubstituted C1-C30 alkoxy groups, and substituted or unsubstituted C6-C60 aryl groups; R2 is selected from substituted or unsubstituted polyethers, substituted or unsubstituted C1-C30 alkyl groups, substituted or unsubstituted C1-C30 alkoxy groups, substituted or unsubstituted C6-C60 aryl groups, and *-b1-SS-b2-*, where b1 and b2 are each independently selected from substituted or unsubstituted C2-C15 linear alkyl groups or substituted or unsubstituted C6-C60 aryl groups; and R3 is an ion-containing liquid group. Due to its special molecular structure, the polymer exhibits excellent electrochemical properties and mechanical strength when applied to complex electrolytes.

Description

Field of Technology

[0001] Embodiments of this application relate to polymers and their use, and belong to the field of energy technology. [Background technology]

[0002] Inorganic solid electrolytes are considered to have broad market potential in batteries due to their excellent ionic conductivity, high energy density, high mechanical strength, and high safety. However, inorganic solid electrolytes are said to be highly brittle and lack flexibility. Features Furthermore, the manufacturing process is complex. In addition, the internal resistance of solid-state batteries is high because the contact at the interface between the inorganic solid electrolyte and the battery's electrode plates is extremely poor.

[0003] Inorganic solid electrolytes Problems due to characteristics In order to overcome, connection This technology involves introducing a polymer electrolyte into an inorganic solid electrolyte to produce an organic-inorganic solid composite electrolyte. Because the polymer possesses excellent flexibility and processability, the resulting organic-inorganic solid composite electrolyte has relatively good flexibility and processability. However, polymer electrolytes have low mechanical strength, poor ionic conductivity at room temperature, and low ion mobility, among other drawbacks. It has characteristics These factors can affect the mechanical and electrochemical properties of organic-inorganic solid composite electrolytes. Furthermore, poor interfacial compatibility between the polymer electrolyte and the inorganic solid electrolyte is a common problem in organic-inorganic solid composite electrolytes, which affects the overall performance of the composite electrolyte. [Overview of the Initiative] [Problems that the invention aims to solve]

[0004] This application provides a polymer that, due to its special molecular structure, exhibits excellent electrochemical properties and mechanical strength when applied to a composite electrolyte.

[0005] This invention provides a composite electrolyte exhibiting excellent electrochemical performance and mechanical strength, which can be widely applied to batteries and improve the overall performance of batteries.

[0006] This application provides a separator comprising the above-mentioned polymer or composite electrolyte, which, when applied to a battery, can improve the overall performance of the battery.

[0007] The battery according to this application contains one of the above-mentioned polymer, composite electrolyte, and separator, and therefore possesses excellent integrated performance. [Means for solving the problem]

[0008] The present invention provides a polymer comprising a first block shown in Formula 1 and a second block shown in Formula 2. [ka] In the formula, R1 is selected from substituted or unsubstituted C1-C30 alkyl groups, substituted or unsubstituted polyethers, substituted or unsubstituted C1-C30 alkoxy groups, and substituted or unsubstituted C6-C60 aryl groups. R2 is selected from substituted or unsubstituted polyethers, substituted or unsubstituted C1-C30 alkyl groups, substituted or unsubstituted C1-C30 alkoxy groups, substituted or unsubstituted C6-C60 aryl groups, and *-b1-SS-b2-*. b1 and b2 are each independently selected from substituted or unsubstituted C2-C15 linear alkyl groups or substituted or unsubstituted C6-C60 aryl groups. R3 is an ion-containing liquid group, m ≥ 1 and n ≥ 1, and both are integers.

[0009] The above polymer satisfies at least one of a) to b) when the polymer contains multiple first blocks of formula 1. a) R3 in multiple first blocks is selected from the same ionic liquid group. b) R1 in multiple first blocks is selected from the same element.

[0010] When the polymer contains a plurality of second blocks of Formula 2, R1 in the plurality of second blocks is selected from the same group, and R2 in the plurality of second blocks is selected from the same group.

[0011] As the above polymer, R3 is selected from one of an imidazole-based ionic liquid group, a pyridine-based ionic liquid group, a quaternary ammonium-based ionic liquid group, or a quaternary phosphonium-based ionic liquid group.

[0012] As the above polymer, R3 is selected from any one of the following groups. [Chemical formula] In the formula, R4 is selected from substituted or unsubstituted C1-C30 alkyl and substituted or unsubstituted C1-C30 alkoxy, R5 is selected from substituted or unsubstituted C1-C10 alkyl, and A is BF4 - , PF6 - , TFSI - , OTf - , DCA - or TOS - selected from.

[0013] As the above polymer, at least one of a) to b) is satisfied. a) R1 in the first block is a chain structure, b) R2 in the second block contains a cyclic structure.

[0014] As the above polymer, The polymer is performing a first reaction on an amino ionic liquid and a diisocyanate-based compound to obtain a first intermediate compound, and performing a second reaction on the first intermediate compound, a diamine-based compound, and a diisocyanate-based compound to obtain a polymer, and is prepared by a method including these steps.

[0015] This application provides a composite electrolyte comprising an inorganic solid electrolyte and the above-mentioned polymer.

[0016] Based on the total mass of the composite electrolyte, the polymer content is 10-30%.

[0017] The above-mentioned composite electrolyte further contains a lithium salt, and the mass percentage content of the lithium salt is 1-10% based on the total mass of the composite electrolyte.

[0018] The above-mentioned composite electrolyte further contains plastic crystals, and the mass percentage content of the plastic crystals is 1-10% based on the total mass of the composite electrolyte.

[0019] This application provides a porous substrate and a separator comprising the polymer or composite electrolyte described above, which is installed on at least a portion of the surface of the porous substrate and / or at least a portion of the voids of the porous substrate.

[0020] This application provides a battery which comprises the above polymer, Alternatively, it may contain the above-mentioned complex electrolytes, Alternatively, it includes the separator described above. [Effects of the Invention]

[0021] The polymer relating to this application includes the structural formulas shown in Formula 1 and Formula 2, and when applied to a composite electrolyte (including an inorganic solid electrolyte and a polymer electrolyte), it can improve the electrochemical and mechanical properties of the composite electrolyte.

[0022] The composite electrolyte according to this application contains a polymer with the special molecular structure described above, and the composite electrolyte possesses excellent electrochemical performance and mechanical strength, making it widely applicable to batteries, improving the electrochemical performance of batteries and extending their service life.

[0023] The separator according to this application contains the above-mentioned polymer or composite electrolyte, and therefore, when applied to a battery, it can improve the electrochemical performance of the battery and extend the battery's service life.

[0024] The battery according to this application contains one of the above-mentioned polymer, composite electrolyte, and separator, and therefore possesses excellent electrochemical performance and a long service life. [Brief explanation of the drawing]

[0025] [Figure 1] This is a measurement curve diagram of the polymer in Example 2 of the present application, obtained by infrared spectroscopy. [Modes for carrying out the invention]

[0026] To clarify the purpose, technical solutions, and advantages of the embodiments of this application, the technical solutions will be described clearly and completely below with reference to the drawings relating to the embodiments of this application. Naturally, the embodiments described are only a part of the examples of this application, not all of them. All other examples obtained by a person skilled in the art without creative work based on the embodiments of this application shall all be within the scope of protection of this application.

[0027] In a first aspect, the present application provides a polymer comprising a first block shown in Formula 1 and a second block shown in Formula 2. [ka] In the formula, R1 is selected from substituted or unsubstituted C1-C30 alkyl groups, substituted or unsubstituted polyethers, substituted or unsubstituted C1-C30 alkoxy groups, and substituted or unsubstituted C6-C60 aryl groups. R2 is selected from substituted or unsubstituted polyethers, substituted or unsubstituted C1-C30 alkyl groups, substituted or unsubstituted C1-C30 alkoxy groups, substituted or unsubstituted C6-C60 aryl groups, and *-b1-SS-b2-*. b1 and b2 are each independently selected from substituted or unsubstituted C2-C15 linear alkyl groups or substituted or unsubstituted C6-C60 aryl groups. R3 is an ion-containing liquid group, m≧1 and n≧1.

[0028] The polymer relating to this application includes a first block shown in Formula 1 and a second block shown in Formula 2. This application does not limit the number of first blocks and second blocks in the polymer; the number of first blocks and second blocks may be the same or different. This application also does not limit the arrangement of the first blocks and second blocks; the first blocks and second blocks may be arranged sequentially (for example, the polymer's structural formula may include sequentially connected first blocks, first blocks, second blocks, and second blocks); the first blocks and second blocks may be arranged alternately (for example, the polymer's structural formula may include sequentially connected first blocks, second blocks, first blocks, and second blocks); or the first blocks and second blocks may be arranged irregularly (for example, the polymer's Structural formula (This may include a sequentially connected first block, second block, first block, first block, second block).

[0029] Specifically, R1 is selected from substituted or unsubstituted polyethers (e.g., substituted linear polyethers, unsubstituted linear polyethers, substituted cyclic polyethers, unsubstituted cyclic polyethers), substituted or unsubstituted C1-C30 alkyl groups (e.g., unsubstituted linear alkyl groups, unsubstituted branched alkyl groups, unsubstituted cyclic alkyl groups, substituted linear alkyl groups, substituted branched alkyl groups, substituted cyclic alkyl groups), substituted or unsubstituted C1-C30 alkoxy groups (e.g., substituted linear alkoxy groups, unsubstituted linear alkoxy groups, substituted cyclic alkoxy groups, unsubstituted cyclic alkoxy groups), and substituted or unsubstituted C6-C60 aryl groups (e.g., substituted phenyl groups, substituted biphenyl groups, unsubstituted phenyl groups, unsubstituted biphenyl groups). R2 is a substituted or unsubstituted C1-C30 alkyl (e.g., unsubstituted linear alkyl, unsubstituted branched alkyl, unsubstituted cyclic alkyl, substituted linear alkyl, substituted branched alkyl, substituted cyclic alkyl), a substituted or unsubstituted C1-C30 alkoxy (e.g., substituted branched alkoxy, substituted linear alkoxy, substituted cyclic alkoxy, unsubstituted linear alkoxy, unsubstituted branched alkoxy, unsubstituted cyclic alkoxy), a substituted or unsubstituted polyether (e.g., Examples include substituted linear polyethers, unsubstituted linear polyethers, substituted cyclic polyethers, and unsubstituted cyclic polyethers), substituted or unsubstituted C6-C60 aryls (e.g., substituted phenyls, substituted biphenyls, unsubstituted phenyls, and unsubstituted biphenyls), and selected from *-b1-SS-b2-* (where b1 and b2 are independently selected from substituted or unsubstituted C2-C15 linear alkyls or substituted or unsubstituted aryls, and * indicates the connection position to the main chain of formula 1 (or formula 2)). This application does not particularly limit the substituents at R1 and R2, and the substituents may be substituents commonly used in the art. Exemplary substituents may be selected from substituted or unsubstituted C1-C30 alkyl groups, substituted or unsubstituted C2-C30 alkenes, substituted or unsubstituted C3-C30 alkynes, esters, substituted or unsubstituted C1-C30 alkoxy groups, substituted or unsubstituted C6-C60 aryl groups, halogens, and amino groups.

[0030] In R3, an ionic liquid group refers to an organic group containing both a cation and anion.

[0031] m and n are positive integers. The polymer according to this application can be compounded with an inorganic solid electrolyte to produce a composite electrolyte containing a polymer electrolyte and an inorganic solid electrolyte. The ionic liquid groups in the polymer according to this application have excellent ionic conductivity, enabling high-speed ion transfer in the composite electrolyte. In addition, the urea (-NH-CO-NH-) in the polymer has a strong polarity effect, generating a strong physical interaction between the polymer electrolyte and the inorganic solid electrolyte, tightly bonding the inorganic solid electrolyte and the polymer electrolyte, and improving the interfacial compatibility between the inorganic solid electrolyte and the polymer electrolyte. Furthermore, the polymer according to this application is a polymer with a substantially block structure, comprising a first block containing ionic liquid groups and a second block containing urea groups. The first block containing ionic liquid groups can improve the conductivity of lithium ions in the polymer electrolyte, and the second block containing urea and the inorganic solid electrolyte exhibit excellent interfacial interaction, reducing the internal interfacial resistance of the composite electrolyte, improving the conductivity of lithium ions between the composite electrolytes, and consequently improving the electrochemical performance of the composite electrolyte.

[0032] Furthermore, the urea atoms within the polymer exhibit strong hydrogen bonding, and a vast dynamic hydrogen bonding network exists within the composite electrolyte containing this polymer. This dynamic hydrogen bonding network continuously opens and closes repeatedly during the deformation process, dissipating the energy generated by the material's deformation and thus imparting excellent mechanical flexibility to the composite electrolyte. Notably, the ionic liquid groups within the polymer also possess excellent flame retardant properties, significantly improving the flame retardancy of the composite electrolyte and, consequently, enhancing the safety performance of the battery.

[0033] In the polymer relating to this application, R1 in the first block and R1 in the second block may be the same or different. When the polymer contains multiple first blocks (m≧2), R1 in the multiple first blocks may be the same or different, and R3 in the multiple first blocks may be the same or different. When the polymer contains multiple second blocks (n≧2), R1 in the multiple second blocks may be the same or different, and R2 in the multiple second blocks may be the same or different.

[0034] In some embodiments of the present invention, when the polymer contains multiple first blocks shown in Formula 1 (m≧2), R3 in the multiple first blocks is selected from the same ionic liquid group, and the same ionic liquid group improves the uniformity of conduction and contributes to imparting high ionic conductivity to the polymer.

[0035] In some embodiments of the present invention, when the polymer contains multiple first blocks shown in Formula 1 (m≧2), R1 in the multiple first blocks is selected from the same group, and the same group contributes to improving the regularity of the polymer, thereby further improving the uniformity and stability of ion conduction.

[0036] In some embodiments of the present invention, when the polymer contains multiple second blocks shown in formula 2 (n≧2), R1 in the multiple second blocks is selected from the same group, R2 is selected from the same group, and the same group contributes to increasing the uniformity of the second block structure, thereby increasing the uniform distribution of interaction sites between molecular chains of the polymer and contributing to improving the physical properties of the polymer.

[0037] In some embodiments of the present application, R3 is selected from one of the following: an imidazole-based ionic liquid group, a pyridine-based ionic liquid group, a quaternary ammonium-based ionic liquid group, or a quaternary phosphonium-based ionic liquid group.

[0038] In the present application, when the polymer containing the ionic liquid group is applied to a composite electrolyte, the ionic conductivity and flame retardant performance at room temperature become more excellent. The ionic liquid for forming the ionic liquid group is easily available and has a relatively low price, which helps to reduce the manufacturing cost.

[0039] Furthermore, R3 is selected from any one of the following groups.

Chemical formula

[0040] Specifically, * in the above structural formula refers to the position interconnected with the main chain shown in Formula 1.

[0041] R4 is selected from a substituted or unsubstituted C1-C30 alkyl (for example, substituted linear alkyl, substituted branched alkyl, substituted cyclic alkyl, unsubstituted branched alkyl, unsubstituted linear alkyl or unsubstituted cyclic alkyl), a substituted or unsubstituted C1-C30 alkoxy (for example, substituted linear alkoxy, substituted cyclic alkoxy, substituted branched alkoxy, unsubstituted cyclic alkoxy, unsubstituted linear alkoxy, unsubstituted branched alkoxy), and R5 is selected from a substituted or unsubstituted C1-C10 alkyl (for example, substituted linear alkyl, substituted branched alkyl, substituted cyclic alkyl, unsubstituted branched alkyl, unsubstituted linear alkyl or unsubstituted cyclic alkyl).

[0042] The formation of anionic groups is obtained by the dissociation of the corresponding salts. For example, the borate tetrafluoride ion is obtained by the dissociation of lithium borate tetrafluoride, and the phosphate hexafluoride ion is obtained by the dissociation of lithium phosphate hexafluoride. The structures of each anionic group in this application are as follows. [ka]

[0043] This application does not particularly limit the substituents in R4 and R5, and the substituents may be substituents commonly used in the art. Exemplary examples, the substituents may be selected from at least one of substituted or unsubstituted C1-C30 alkyl groups, substituted or unsubstituted C2-C30 alkenes, substituted or unsubstituted C3-C30 alkynes, esters, substituted or unsubstituted C1-C30 alkoxy groups, substituted or unsubstituted C6-C60 aryl groups, and halogens.

[0044] When R3 is selected from the above structural formula, it becomes possible to improve the electrochemical performance and flame retardancy of the battery while reducing manufacturing costs.

[0045] In some embodiments of the present application, R1 in the first block is a chain structure. That is, R1 in the first block is selected from substituted or unsubstituted chain polyethers, substituted or unsubstituted chain C1-C30 alkyl groups, and substituted or unsubstituted chain C1-C30 alkoxy groups.

[0046] When R1 in the first block has a chain-like structure, the lithium ion transfer performance between ionic liquid structures can be adjusted, thereby improving the lithium ion transfer efficiency of the composite electrolyte.

[0047] In some embodiments of the present application, R2 in the second block has a cyclic structure. That is, R2 in the second block is selected from substituted or unsubstituted cyclic polyethers, substituted or unsubstituted C6-C60 aryls, *-b1-SS-b2-* (where b1 and b2 are independently selected from substituted or unsubstituted C6-C60 aryls), substituted or unsubstituted cyclic C3-C30 alkyls, and substituted or unsubstituted cyclic C3-C30 alkoxys.

[0048] When R2 in the second block has a cyclic structure, it contributes to improving the rigidity and thermal performance of the polymer, thereby improving the mechanical and heat-resistant properties of the composite electrolyte and extending the battery's lifespan.

[0049] In particular, when R1 in the first block of the polymer has a chain structure and R2 in the second block has a cyclic structure, the structural formula of the polymer possesses both rigidity and flexibility. This not only contributes to improving the physical performance of the second block, but also enhances the flexibility of the molecular chain structure of the second block, allowing for morphological adjustment of the molecular chains during interaction with the inorganic solid electrolyte. This contributes to an increase in the interaction sites between the second block and the inorganic solid electrolyte particles, improving the interfacial bonding performance between the polymer and the inorganic solid electrolyte. This reduces the internal interfacial resistance of the composite solid electrolyte, resulting in the polymer electrolyte possessing excellent mechanical and lithium-ion conductivity. Consequently, it improves the electrochemical performance of the battery and extends its lifespan.

[0050] This application does not impose any special restrictions on the raw materials and manufacturing methods for the polymer. As long as the polymer satisfies the above-mentioned characteristics, the raw materials and manufacturing methods can be freely selected according to the purpose.

[0051] In some embodiments of this application, the polymer is A first reaction is carried out with an amino ionic liquid and a diisocyanate compound to obtain a first intermediate compound, The polymer is prepared by a method comprising the steps of carrying out a second reaction with a first intermediate compound, a diamine compound, and a diisocyanate compound to obtain a polymer.

[0052] Specifically, the polymer is produced by carrying out a first reaction with an amino ionic liquid and a diisocyanate compound, in which the amino in the amino ionic liquid reacts with the isocyanate in the diisocyanate compound to form a first intermediate compound containing a first block, the R3 group in the first block originates from the amino ionic liquid, and the R1 group in the first block originates from the diisocyanate compound. The present invention involves a second reaction with a first intermediate compound, a diamine compound, and a diisocyanate compound, wherein in the second reaction, the amino in the diamine compound reacts with the isocyanate in the diisocyanate compound to form a second block containing urea, while the second block bonds with the first intermediate compound to form a polymer containing the first and second blocks, wherein the R1 group in the second block is derived from the diisocyanate compound, and the R2 group in the second block is derived from the diamine compound.

[0053] This application does not particularly limit the amino ionic liquid, and any amino ionic liquid commonly used in this field may be used. The amino ionic liquid may be purchased commercially or obtained by preparing it in the laboratory.

[0054] This application does not particularly limit diisocyanate compounds. Diisocyanate compounds may be compounds containing two isocyanates, which are commonly used in the art. Examples of diisocyanate compounds include polyethylene glycol diisocyanate, isophorone diisocyanate, hexamethylene diisocyanate, 4,4'-diphenylmethane diisocyanate, 1,4-phenylenediisocyanate, 1,4-diisocyanatebutane, 1,3-phenylene diisocyanate, 1,12-diisocyanatododecane, toluene diisocyanate-polypropylene glycol copolymer, 1,6-diisocyanate-2,2,4-trimethylhexane, 2,6-diisocyanate methylbenzene ester, and 6-(4-isocyanatephenoxy)-hexane. Acid, 2 -[6-(4-isocyanate phenoxy)-hexanoyloxy]-ethyl ester, m-xylylene diisocyanate, toluene-2,4-diisocyanate, and dicyclohexylmethane 4,4'-diisocyanate may be selected from at least one of these.

[0055] The present application does not particularly limit diamine compounds, and may include compounds containing two amino acids in the art. For example, diamine compounds may be selected from at least one of polyetheramine, cysteinamine, bis(3-aminopropyl) disulfide, 4,4'-diaminodicyclohexylmethane, hexamethylenediamine, 4,7,10-trioxo-1,13-tridecanediamine, 4,4'-diaminodiphenylmethane, paraphenylenediamine, polyethylene glycol diamine, 4,9-dioxo-1,12-dodecanediamine, 4,4'-diaminodiphenyl disulfide, di(6-aminohexyl) disulfide, and 0,0'-di(2-aminopropyl)polypropylene glycol-block-polyethylene glycol-block-polypropylene glycol.

[0056] This application does not limit the order in which the starting materials are added in the second reaction. The first intermediate compound, the diamine compound, and the diisocyanate compound may be mixed first, and then the second reaction may be initiated; or the diamine compound and the diisocyanate compound may be mixed first, and then added to the first intermediate compound to initiate the second reaction; or the first intermediate compound and the diamine compound may be mixed first, and then the diisocyanate compound may be added to initiate the second reaction.

[0057] The present invention does not particularly limit the specific parameters of the first reaction, as long as the amino in the amino ionic liquid can react with the isocyanate in the diisocyanate compound. In some embodiments, the temperature in the first reaction is 0 to 10°C and the time is 5 to 180 minutes.

[0058] The present invention does not particularly limit the specific parameters of the second reaction, as long as the amino in the diamine compound can react with the isocyanate in the diisocyanate compound and the second block can bond with the first block. In some embodiments, the temperature in the second reaction is 0 to 10°C and the time is 5 to 300 minutes.

[0059] In some embodiments, polymers can be produced by a method comprising the steps of: reacting an amino ionic liquid with a diisocyanate compound at 0-10°C for 5-180 minutes to obtain a first intermediate compound; and gradually adding a diamine compound, then gradually adding another diisocyanate compound, and reacting them at 0-10°C for 5-300 minutes.

[0060] This invention does not particularly limit the amount of each raw material to be added and can be selected according to actual needs. In some embodiments, if an excess of the diisocyanate compound is present in the first reaction, a complete chemical reaction can occur with the amino acids in the amino ionic liquid, thereby forming a first block structure. Alternatively, if an excess of the diisocyanate compound is present, a first intermediate compound having reactive isocyanate groups at both ends can be obtained, allowing the first intermediate compound to directly undergo the second reaction. In the second reaction, by adjusting the molar ratio of the first intermediate compound, the diamine compound, and the diisocyanate compound, and making the molar content of isocyanate and amino acids nearly equal, the change in the molecular weight distribution of the polymer can be appropriately controlled, preventing an excess of isocyanate or amino acids from significantly affecting the degree of polymerization of the polymer and causing an excessive change in the molecular weight distribution, thereby affecting the physical properties of the polyurethane polymer.

[0061] Furthermore, in some embodiments, in the first reaction, the molar ratio of the amino ionic liquid to the diisocyanate compound is 1:(2.0~2.1), and in the second reaction, the molar ratio of the first intermediate compound to the diamine compound to the diisocyanate compound is 1:(1.5~1.7):(0.5~0.6), meaning that in the second reaction, the molar ratio of isocyanate to amino is approximately 1:(1.0~1.1).

[0062] This invention not only provides a polymer with excellent integrated performance by producing a polymer using the above manufacturing method, but also demonstrates that the manufacturing method is easy to operate and suitable for large-scale production.

[0063] In a second aspect, the present application provides a composite electrolyte comprising an inorganic solid electrolyte and a polymer according to the first aspect of the present application.

[0064] This application does not particularly limit the inorganic solid electrolyte, and the inorganic solid electrolyte may be any inorganic solid electrolyte commonly used in this field. For example, the inorganic solid electrolyte may be selected from at least one of lithium lanthanum zirconium oxygen (LLZO), lithium lanthanum zirconium tantalum oxygen (LLZTO), titanium aluminum lithium phosphate (LATP), and germanium aluminum lithium phosphate (LAGP).

[0065] In this application, the polymer can form a polymer electrolyte, thereby the composite electrolyte will contain both an inorganic solid electrolyte and a polymer electrolyte.

[0066] In composite electrolyte membranes manufactured using existing technologies, the polymer of the polymer electrolyte is typically polypropylene nitrile (PAN), polyoxyethylene (PEO), polyvinylidene fluoride (PVDF), and polymethyl methacrylate (PMMA). The ionic conductivity and mechanical strength of such composite electrolytes are relatively low. In addition, the interfacial compatibility between the polymer electrolyte and the inorganic solid electrolyte is poor, resulting in significant interfacial resistance within the composite electrolyte, which affects the transfer of lithium ions between the polymer electrolyte and the inorganic solid electrolyte. As a result, the electrochemical performance of the composite electrolyte deteriorates. Compared to existing technologies, the composite electrolyte according to the present invention contains a polymer having a special structure as described in the first embodiment and an inorganic solid electrolyte, possessing excellent ionic conductivity and mechanical strength. Furthermore, because the interfacial compatibility between the polymer electrolyte and the inorganic solid electrolyte in the composite electrolyte is excellent, the composite electrolyte can significantly improve the electrochemical performance of the battery and extend its service life.

[0067] Furthermore, in some embodiments of the present invention, if the mass percentage content of the polymer is 10-30% and the mass percentage content of the inorganic solid electrolyte is greater than 0% and 90% or less, based on the total mass of the composite electrolyte, it is possible to maximize the function of the polymer while suppressing the consumption of the polymer and improving the total mass of the composite electrolyte.

[0068] In some embodiments of the present application, the composite electrolyte further comprises a lithium salt, and the mass percentage content of the lithium salt is 1 to 10% based on the total mass of the composite electrolyte.

[0069] When the composite electrolyte further contains a lithium salt, the lithium salt better composites with the polymer to form a polymer electrolyte, and a composite electrolyte containing a polymer electrolyte and an inorganic solid electrolyte can be obtained. This composite electrolyte has superior ion mobility and ionic conductivity. In particular, when the mass percentage content of the lithium salt in the composite electrolyte is 1 to 10%, the ion mobility and ionic conductivity of the composite electrolyte can be improved by further enhancing the interaction between the lithium salt and the polymer while suppressing the consumption of lithium salt.

[0070] In some embodiments, the composite electrolyte exhibits superior overall performance when the mass percentage content of the polymer in the composite electrolyte is 10-30%, the mass percentage content of the lithium salt is 1-10%, and the mass percentage content of the inorganic solid electrolyte is 60-89%.

[0071] This application does not particularly limit the lithium salt, and any lithium salt commonly used in the art may be used. For example, the lithium salt may be selected from at least one of bis(trifluoromethanesulfonyl)imide lithium (LiTFSI), difluoro(oxalato)borate lithium (LiDFOB), hexafluorophosphate lithium (LiPF6), tetrafluoroborate lithium (LiBF4), lithium bis(oxalato)borate (LiBOB), and lithium bis(fluorosulfonyl)imide (LiFSI).

[0072] Please understand that this invention allows for both the direct addition of lithium salts during the manufacturing process of the composite electrolyte and the addition of lithium salts in the form of an electrolyte during the manufacturing process of the battery.

[0073] In some embodiments of the present application, the composite electrolyte further comprises plastic crystals, and the mass percentage content of the plastic crystals is 1 to 10% based on the total mass of the composite electrolyte.

[0074] This application does not particularly limit the plastic crystal, and the plastic crystal may be any plastic crystal commonly used in this field. For example, the plastic crystal may be succinonitrile.

[0075] This invention utilizes the excellent physical interaction between succinonitrile and electron-rich components (e.g., oxygen element, ester, etc.) in the composite electrolyte to strengthen the dynamic bonding network structure in the composite electrolyte, thereby imparting excellent physical and mechanical strength to the composite electrolyte. In addition, the use of succinonitrile further improves the interfacial bonding between the organic electrolyte and the inorganic solid electrolyte, reducing the internal resistance of the composite solid electrolyte and promoting lithium ion transfer at the interface. Furthermore, the strong polarity of succinonitrile and polyurethane exhibits excellent adsorption to anionic groups, suppressing the movement of anionic groups in the composite electrolyte, reducing the resistance to lithium ion transfer in the composite electrolyte, and enabling high-speed transfer. Moreover, if the mass percentage content of plastic crystals in the composite electrolyte is 1-10%, the consumption of plastic crystals can be reduced while further improving the interaction between the plastic crystals and the lithium salt and / or inorganic solid electrolyte, thereby improving the overall performance of the composite electrolyte. In some embodiments, the composite electrolyte exhibits superior integrated performance when the mass percentage content of the polymer in the composite electrolyte is 10-30%, the mass percentage content of the inorganic solid electrolyte is 50-88%, the mass percentage content of the plastic crystal is 1-10%, and the mass percentage content of the lithium salt is 1-10%.

[0076] This application does not impose any special restrictions on the method of manufacturing the composite electrolyte, and those skilled in the art can freely select a manufacturing method according to their purpose.

[0077] In this invention, the composite electrolyte can be manufactured by forming a self-supporting membrane. Examples include a method in which the raw material system is poured onto a release membrane, solidified to form a membrane, and then peeled off, or a method in which the raw material system is extruded to form a membrane.

[0078] In some embodiments, the composite electrolyte is prepared by a method comprising the steps of: adding an inorganic solid electrolyte to a first solvent to obtain a first mixture; adding a polymer to a second solvent to obtain a second mixture; completely mixing the first and second mixtures to obtain a third mixture; and pouring the third mixture onto the surface of a release film as a raw material system, after which the first and second solvents are removed and the mixture is separated from the release film to obtain the composite electrolyte.

[0079] This application does not impose any special restrictions on the first and second solvents, and they can be selected from commonly used solvents, such as N-methylpyrrolidone (NMP), acetone, methanol, and ethanol.

[0080] In some embodiments, the method for producing a composite electrolyte may further include the step of adding a lithium salt to a third mixture obtained by completely mixing a first mixture and a second mixture, and stirring thoroughly to obtain a uniformly mixed raw material system.

[0081] In some embodiments, the method for producing a composite electrolyte may further include the step of adding a lithium salt and plastic crystals to a third mixture obtained by completely mixing a first mixture and a second mixture, and stirring thoroughly to obtain a uniformly mixed raw material system.

[0082] In a third aspect, the present invention provides a separator comprising a porous substrate and a polymer according to the first aspect or a composite electrolyte according to the second aspect, which is installed on at least a portion of the surface of the porous substrate and / or at least a portion of the voids of the porous substrate.

[0083] In the separator according to this application, the polymer may be placed on a part or the entire surface of the porous substrate, or on a part or the entire void of the porous substrate, and the composite electrolyte may be placed on a part or the entire surface of the porous substrate, or on a part or the entire void of the porous substrate.

[0084] This invention does not limit the specific installation method, and a separator can be formed by employing installation methods commonly used in the art, and by installing a polymer or composite electrolyte on at least a portion of the surface of a porous substrate and / or at least a portion of the voids of the porous substrate.

[0085] In some embodiments, a separator can be obtained by coating a polymer or composite electrolyte raw material system onto a porous substrate and allowing it to solidify. Alternatively, a separator can be obtained by compounding a self-film-forming polymer or composite electrolyte with a porous substrate by hot-pressure or roll-rolling, and the porous substrate may be any porous substrate commonly used in battery separators. For example, the porous substrate may be a film or woven substrate formed from any of the following polymers, and the polymer may be selected from at least one of polyethylene terephthalate, polybutylene terephthalate, polymethyl methacrylate, polyacetal, polyamide, polycarbonate, polyimide, polyetheretherketone, polyethersulfone, polyphenylene ether, polyphenylene sulfide, polyethylene naphthalate, polyvinylidene fluoride, polyethylene oxide, polyacrylonitrile, tetrafluoropropene copolymer, hexafluoropropene copolymer, or from at least one of copolymers of propylene, 1-butene, pentene, 1-hexene, 4-methyl-1-pentene, 1-octene, 1-decene, homogeneous polymers and their derivatives.

[0086] In some embodiments, the product is prepared by a method comprising the steps of: adding an inorganic solid electrolyte to a first solvent to obtain a first mixture; adding a polymer to a second solvent to obtain a second mixture; completely mixing the first and second mixtures to obtain a third mixture; and applying the third mixture as a raw material system to at least a portion of the surface of a porous substrate, and then heating and drying it to remove the first and second solvents to obtain a separator.

[0087] This application does not impose any special restrictions on the first and second solvents, and they can be selected from commonly used solvents, such as N-methylpyrrolidone (NMP), acetone, methanol, and ethanol.

[0088] In some embodiments, the method for manufacturing the separator may further include the step of adding a lithium salt to a third mixture obtained by completely mixing a first mixture and a second mixture, and stirring thoroughly to obtain a uniformly mixed raw material system.

[0089] In some embodiments, the method for manufacturing the separator may further include the step of adding a lithium salt and plastic crystal to a third mixture obtained by completely mixing a first mixture and a second mixture, and stirring thoroughly to obtain a uniformly mixed raw material system.

[0090] In some embodiments, the method for manufacturing the separator may further include a step of roll-rolling the separator obtained after drying to further strengthen the bond between the polymer or composite electrolyte and the porous substrate.

[0091] Since the separator according to this application contains the above-mentioned polymer or composite electrolyte, when applied to a battery, it can improve the electrochemical performance of the battery and expand the range of battery applications.

[0092] In a fourth aspect, the present application provides a battery which comprises the polymer in the first aspect, Alternatively, it may include a composite electrolyte in the second embodiment, Alternatively, it includes a separator in a third embodiment.

[0093] Please understand that the battery relating to this application further comprises a positive electrode plate, a negative electrode plate, and a package.

[0094] In this invention, a positive electrode plate, a composite electrolyte (or separator), and a negative electrode plate are stacked and arranged to obtain an electrode assembly, the electrode assembly is placed in a package, and a battery is obtained by sealing it.

[0095] Because the battery according to this application contains the above-mentioned composite electrolyte, it possesses excellent electrochemical performance, offers a superior user experience, and is suitable for widespread application.

[0096] The technical measures related to this application will be described in detail below using specific examples. [Examples]

[0097] The origins of some of the components in the examples and comparative examples are as follows. For components in the examples or comparative examples where specific experimental procedures or conditions are not specified, these components can be obtained by following the usual experimental procedures or conditions described in existing art.

[0098] (1) Aminoionic liquid: 1-Aminopropyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (CAS: 1013932-26-7) 1-Aminoethyl-3-methylimidazole tetrafluoroborate (CAS: 897965-53-6), All of the above amino ion liquids were purchased from Qingdao Aolike New Materials Technology Co., Ltd.

[0099] (2) Diisocyanate compounds: Hexamethylene diisocyanate (CAS: 822-06-0), Diphenylmethane-4,4'-diisocyanate (CAS: 101-68-8) 1,12-Diisocyanatododecane (CAS: 13879-35-1), All of the above diisocyanate compounds were purchased from Shanghai Alading Biochemical Technology Co., Ltd.

[0100] (3) Diamine compounds: Polyetheramine D230 (CAS: 9046-10-0), 2,2'-Dithiodiethylamine (CAS: 56-17-7), 4,4'-Diaminodicyclohexylmethane (CAS: 1761-71-3) All of the above diamine compounds were purchased from Shanghai Malcolm Biochemical Technology Co., Ltd.

[0101] (4) Plastic crystal materials: Sucinonitrile (CAS: 110-61-2) All of the above plastic crystal materials were purchased from Shanghai McLin Biochemical Technology Co., Ltd.

[0102] Example 1 The battery in this embodiment is manufactured by a method that includes the following steps.

[0103] 1) Preparation of polymers The process includes the steps of: carrying out a first reaction with an amino ionic liquid and a diisocyanate compound to obtain a first intermediate compound; and then gradually adding a diamine compound, followed by gradually adding another diisocyanate compound, to carry out a second reaction and obtain a polymer. The amino ionic liquid is 1-aminopropyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide, the diisocyanate compound is hexamethylene diisocyanate, and the diamine compound is 4,4'-diaminodiphenylmethane. In the first reaction, the molar ratio of the amino ionic liquid to the diisocyanate compound was 1:1.05, the reaction temperature was 5°C, and the reaction time was 120 minutes. In the second reaction, the molar ratio of the first intermediate product to the diisocyanate compound and the diamine compound is 1:1.5:0.5. The reaction temperature is 5°C and the reaction time is 240 minutes.

[0104] 2) Preparation of composite electrolytes A step of dispersing an inorganic solid electrolyte in an NMP solvent to obtain a first dispersion, Step 1) involves dissolving the polymer in NMP solvent to obtain a first solution, A step of completely mixing the first dispersion and the first solution to obtain the second solution, Next, succinonitrile and lithium salt are added to the second solution, and the mixture is stirred for 1 hour to obtain a uniformly mixed raw material system. The process includes the steps of applying the raw material system to at least a portion of the surface of a porous substrate, and then heating and drying it to remove the NMP solvent and obtain a composite electrolyte, The inorganic solid electrolyte is LATP, the lithium salt is lithium hexafluorophosphate, and the porous substrate is a PET nonwoven porous membrane. In the composite electrolyte, the mass percentage content is 60% for inorganic solid electrolyte, 5% for lithium salt, 5% for plastic crystal, and 30% for polymer.

[0105] 3) Battery manufacturing The process includes stacking a positive electrode plate, a composite electrolyte, and a negative electrode plate to obtain an electrode assembly, placing the electrode assembly in an aluminum plastic film, and sealing it to obtain a battery. The positive electrode plate includes an aluminum foil and a positive electrode active layer placed on the surface of the aluminum foil. The positive electrode active layer contains lithium cobalt oxide, a conductive agent Super P, and an adhesive PVDF. The mass ratio of lithium cobalt oxide, conductive agent, and adhesive is 96:2:2. The negative electrode plate includes a copper foil and a negative electrode active layer placed on the surface of the copper foil. The negative electrode active layer contains silicon-doped graphite, a conductive agent Super P, and an adhesive PAA. The mass ratio of silicon-doped graphite, conductive agent, and adhesive is 95:2:3.

[0106] Example 2 The method for manufacturing the battery in this embodiment is almost the same as in Example 1, 1) Preparation of polymers The diisocyanate compounds differ in that they are diphenylmethane-4,4'-diisocyanate.

[0107] Example 3 The method for manufacturing the battery in this embodiment is almost the same as in Example 1, 1) Preparation of polymers The diamine compound differs in that it is polyetheramine D230.

[0108] Example 4 The method for manufacturing the battery in this embodiment is almost the same as in Example 1, 1) Preparation of polymers The amino ionic liquid differs in that it is 1-aminoethyl-3-methylimidazole tetrafluoroborate, the diisocyanate compound is 1,12-diisocyanatododecane, and the diamine compound is 2,2'-dithiodiethylamine.

[0109] Example 5 The method for manufacturing the battery in this embodiment is almost the same as in Example 1, 1) Preparation of polymers In the first reaction, the amino ionic liquid is 1-aminoethyl-3-methylimidazole tetrafluoroborate, and the diisocyanate compound is 1,12-diisocyanatododecane, and The second reaction differs in that the diamine compound is polyetheramine D230, and the diisocyanate compound is diphenylmethane-4,4'-diisocyanate.

[0110] Example 6 The method for manufacturing the battery in this embodiment is almost the same as in Example 1, 1) Preparation of polymers In the first reaction, the diisocyanate compounds are hexamethylene diisocyanate and 1,12-diisocyanatododecane (the molar ratio of hexamethylene diisocyanate to 1,12-diisocyanatododecane is 1:1), and The second reaction differs in that the diamine compound is 4,4'-diaminodicyclohexylmethane, while the diisocyanate compound is diphenylmethane-4,4'-diisocyanate.

[0111] Example 7 The method for manufacturing the battery in this embodiment is almost the same as in Example 1, 2) Preparation of composite electrolytes The fact that succinonitrile is not added, and In the composite electrolyte, the difference lies in the fact that the mass percentage content of the inorganic solid electrolyte is 65%, the mass percentage content of the lithium salt is 5%, and the mass percentage content of the polymer is 30%.

[0112] Comparative Example 1 The method for manufacturing the battery in this comparative example is almost the same as in Example 1, 1) Preparation of polymers The polymer was prepared by a one-pot method, by simultaneously adding an amino ionic liquid, a diisocyanate compound, and a diamine compound to a reaction vessel. The molar ratio of the amino ionic liquid, the diisocyanate compound, and the diamine compound is 1:2.1:1.1, and The differences lie in the reaction temperature (5°C) and reaction time (240 minutes).

[0113] Comparative Example 2 The battery manufacturing method in this comparative example is almost the same as that in comparative example 1, 1) Preparation of polymers The diisocyanate compounds differ in that they are diphenylmethane-4,4'-diisocyanate.

[0114] Comparative Example 3 The method for manufacturing the battery in this comparative example is almost the same as in Example 1, 1) Preparation of polymers The advantage is that a polymer is obtained by directly reacting a diisocyanate compound with a diamine compound without containing an amino ionic liquid, and The differences lie in the molar ratio of the diisocyanate compound to the diamine compound (1:1.1), the reaction temperature (5°C), and the reaction time (240 minutes).

[0115] Comparative Example 4 The battery manufacturing method in this comparative example is almost the same as that in comparative example 1, 2) Preparation of composite electrolytes In that no plastic crystal material is added, In the composite electrolyte, the difference lies in the fact that the mass percentage content of the inorganic solid electrolyte is 65%, the mass percentage content of the lithium salt is 5%, and the mass percentage content of the polymer is 30%.

[0116] Performance Test The polymers, composite electrolytes, and batteries in the examples and comparative examples were subjected to the following performance tests, and the test results are shown in Table 1.

[0117] 1. Measurement by infrared spectroscopy Figure 1 is a diagram of the infrared spectroscopy measurement curve of the polymer in Example 2 of the present application. As shown in Figure 1, in the infrared spectroscopy measurement curve of the polymer in Example 2 of the present application, 3304 cm⁻¹ -1 and 1637cm -1 The absorption peaks at 1508 cm² are the stretching vibration absorption of NH and C=O in urea, respectively. -1 1593cm -1 The absorption peak originates from vibrational absorption of the benzene ring, at 3033 cm⁻¹. -1 The absorption peak at 839 cm² is the absorption of stretching vibrations of the CH bond on the benzene ring. -1 The strong absorption peak at 1537 cm⁻¹ originates from the absorption of out-of-plane bending vibrations of the CH bond in the benzene ring, and the benzene ring is 1,4-para substituted. -1 The absorption peak at 1177 cm² originates from the absorption of skeletal vibrations of the imidazole ring. -1 The peak at 2856 cm² is the stretching vibration absorption peak of the imidazole ring. -1 and 2931cm -1 The absorption peaks at this point are the stretching vibration absorption peaks of methyl and methylene, at 1408 cm². -1 The absorption peak at 1230 cm² originates from vibrational absorption of the tertiary amine bond. -1 The absorption peak at 1304 cm originates from the absorption of stretching vibrations of the CN bond. -1 The absorption peak in this region originates from the vibrational absorption of the CN bond in the aromatic amine. This demonstrates that in Example 2 of the present invention, we successfully prepared polymers having the structural formulas shown in Formulas 1 and 2.

[0118] 2. Ionic conductivity at room temperature The measurements were taken according to the method specified in "Method for Measuring Ionic Conductivity of Thin Films in Power Batteries" (Industry Standard NB / T 10827-2021).

[0119] 3. Battery cycle performance The measurements were taken in accordance with the methods specified in the national standard GB / T31486-2015, "Electrical performance requirements and test methods for power storage batteries for electric vehicles."

[0120] 4. Extreme Oxygen Index Measurements were taken in accordance with the methods specified in GB / T2406.1-2008 "Measurement of combustion behavior of plastics by oxygen index method, Part 1: Guidelines" and GB / T2406.2-2009 "Measurement of combustion behavior of plastics by oxygen index method, Part 2: Room temperature test".

[0121] 5. Internal resistance The internal resistance of the battery is characterized according to the electrochemical resistance test methods described in TSPSTS 019-2021 "Performance requirements and test methods for solid electrolytes for solid lithium-ion batteries - Inorganic oxide solid electrolytes" and TSPSTS 020-2021 "Performance requirements and test methods for solid electrolytes for solid lithium-ion batteries - Polymer and composite solid electrolytes".

[0122] 6. Tensile strength The tensile strength of the composite electrolyte was measured according to the standard test method of ASTM D638-14, "Standard Test Method for Tensile Performance of Plastics."

[0123] [Table 1]

[0124] Table 1 shows that the composite electrolyte prepared with polymers in the embodiments of this application exhibits excellent ionic conductivity, critical oxygen index, and tensile strength at room temperature. When this composite electrolyte is applied to a battery, it is confirmed to improve the battery's capacity retention, reduce its internal resistance, and impart excellent overall performance to the battery.

[0125] Furthermore, according to Example 1 and Comparative Example 1, the ionic conductivity of the composite electrolyte (Example 1) prepared with a polymer containing the first block shown in Formula 1 and the second block shown in Formula 2 is superior to that of the composite electrolyte (Comparative Example 1) obtained with a disordered polymer structure. In battery applications, the battery of Example 1 exhibits a better cycle capacity retention rate and lower internal resistance. This demonstrates that polymers with higher regularity and block structure improve the overall performance of the composite electrolyte, thereby contributing to improved overall performance of the battery.

[0126] Finally, it should be noted that the above embodiments are intended to illustrate, and not limit, the technical solutions of the present application. However, the present application will be described in detail with reference to the above embodiments. Those skilled in the art will still be able to modify the technical solutions described in the above embodiments or make equivalent substitutions to some or all of their technical features, and these modifications or substitutions should be understood not to deviate from the essence of the corresponding technical solutions within the scope of the technical solutions of the embodiments of the present application.

Claims

1. A polymer comprising a first block shown in formula 1 and a second block shown in formula 2. 【Chemistry 1】 During the ceremony, R １ These are selected from substituted or unsubstituted C1-C30 alkyl groups, substituted or unsubstituted polyethers, substituted or unsubstituted C1-C30 alkoxy groups, and substituted or unsubstituted C6-C60 aryl groups. R ２ This is selected from substituted or unsubstituted polyethers, substituted or unsubstituted C1-C30 alkyl groups, substituted or unsubstituted C1-C30 alkoxy groups, substituted or unsubstituted C6-C60 aryl groups, and *-b1-S-S-b2-*. b1 and b2 are each independently selected from substituted or unsubstituted C2-C15 linear alkyl groups or substituted or unsubstituted C6-C60 aryl groups. R ３ It is an ion-containing liquid group, m ≥ 1 and n ≥ 1, and both are integers.

2. The polymer according to claim 1, wherein the polymer includes a plurality of first blocks shown in formula 1, and satisfies at least one of a) to b). a) R in multiple of the first blocks ３ These are selected from the same ionic liquid group. b) R in multiple of the first blocks １ They are selected from the same base.

3. When the polymer contains a plurality of second blocks shown in formula 2, R in the plurality of second blocks １ R in multiple of the aforementioned second blocks is selected from the same group. ２ The polymer according to claim 1, which is selected from the same group.

4. The aforementioned R ３ The polymer according to any one of claims 1 to 3, wherein is selected from one of an imidazole-based ionic liquid group, a pyridine-based ionic liquid group, a quaternary ammonium-based ionic liquid group, or a quaternary phosphonium-based ionic liquid group.

5. Said R ３ is the polymer according to claim 4, selected from any one of the following groups. 【Chemistry 2】 During the ceremony, R ４ These are selected from substituted or unsubstituted C1-C30 alkyl groups and substituted or unsubstituted C1-C30 alkoxy groups. R ５ This is selected from substituted or unsubstituted C1-C10 alkyl groups. A is BF ４ － , PF ６ － TFSI － , OTf － DCA － or TOS － They are selected from among them.

6. A polymer according to any one of claims 1 to 5, satisfying at least one of a) to b). a) R in the first block １ It has a chain-like structure. b) R in the second block ２ It includes a ring structure.

7. The aforementioned polymer is A step of performing a first reaction with an amino ionic liquid and a diisocyanate compound to obtain a first intermediate compound, A step of performing a second reaction with the first intermediate compound, a diamine compound, and a diisocyanate compound to obtain the polymer, The polymer according to any one of claims 1 to 6, manufactured by a method comprising the above.

8. A composite electrolyte comprising an inorganic solid electrolyte and a polymer according to any one of claims 1 to 7.

9. The composite electrolyte according to claim 8, wherein, based on the total mass of the composite electrolyte, the mass percentage content of the polymer is 10 to 30%, and the mass percentage content of the inorganic solid electrolyte is greater than 0% and 90% or less.

10. The composite electrolyte according to claim 8 or 9, further comprising a lithium salt, wherein the mass percentage content of the lithium salt is 1 to 10% based on the total mass of the composite electrolyte.

11. The composite electrolyte according to claim 10, further comprising plastic crystals, wherein the mass percentage content of the plastic crystals is 1 to 10% based on the total mass of the composite electrolyte.

12. A separator comprising a porous substrate and a polymer according to any one of claims 1 to 7 or a composite electrolyte according to any one of claims 8 to 11, provided on at least a portion of the surface of the porous substrate and / or at least a portion of the voids of the porous substrate.

13. It is a battery, The polymer comprises the polymer described in any one of claims 1 to 7, Alternatively, it may contain the composite electrolyte described in any one of claims 8 to 11. Alternatively, a battery comprising the separator described in claim 12.

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