Co-crystal electrolyte and preparation method thereof, integrated solid-state negative electrode sheet and solid-state battery

Abstract

The present application relates to the technical field of battery, especially to a eutectic electrolyte, a preparation method thereof, an integrated solid-state negative electrode sheet and a solid-state battery. The eutectic electrolyte comprises raw materials, which include a eutectic precursor, a crosslinking agent and an initiator. The eutectic precursor includes a hydrogen donor, a hydrogen acceptor and an amidosiloxane polymer monomer. The structural formula of the amidosiloxane polymer monomer is: wherein R1, R2 and R3 are each independently any one of an alkyl group, an alkoxy group and a siloxy group. The present application forms a ternary eutectic solid-state electrolyte through the amidosiloxane monomer, a nitrile and a lithium salt, which has high ionic conductivity and ion transmission. The present application is further used for constructing an integrated solid-state negative electrode, forming a high ion channel, improving the interface contact between the electrolyte and the electrode and reducing the interface impedance.

Description

Technical Field

[0001] This invention relates to the field of battery technology, and in particular to eutectic electrolytes and their preparation methods, integrated solid-state anode sheets, and solid-state batteries. Background Technology

[0002] The demand for high-safety, high-energy-density batteries is increasingly urgent in fields such as electric vehicles and large-scale energy storage. As a core component of batteries, the performance of the electrolyte directly affects the overall performance of the battery, making it a key factor for technological breakthroughs. However, traditional electrolytes suffer from the following drawbacks: liquid electrolytes are flammable and have poor thermal stability, easily leading to lithium dendrite growth and thermal runaway; solid electrolytes have high interfacial impedance and insufficient room-temperature ionic conductivity; and ionic liquid electrolytes are expensive and have high viscosity; all of these factors hinder industrial upgrading.

[0003] Eutectic electrolytes are eutectic systems formed by non-covalent interactions between hydrogen bond donors and acceptors. They combine the high ionic conductivity of liquid electrolytes with the high safety of solid electrolytes, while also offering advantages such as tunable structure and lower cost, making them effectively adaptable to high-voltage electrodes and wide-temperature applications. Despite progress in performance optimization, eutectic electrolytes still face the following challenges: Eutectic electrolytes have a higher viscosity than traditional liquid electrolytes, making it difficult to effectively wet the interior of porous electrodes and hindering the construction of continuous ion transport pathways between active material particles, resulting in poor battery performance at high rates. In eutectic electrolyte systems, there is a strong coordination interaction between lithium ions and polar groups (such as cyano and carbonyl groups), resulting in low lithium ion transference numbers. This not only limits the battery's rapid charge and discharge capabilities but also easily leads to concentration polarization within the electrodes, inducing lithium dendrite growth and posing safety hazards. Furthermore, eutectic electrolytes also suffer from insufficient long-term interfacial stability and unclear component-performance structure-activity relationships.

[0004] In view of this, the present invention is hereby proposed. Summary of the Invention

[0005] The primary objective of this invention is to provide a eutectic electrolyte that solves the problems of existing eutectic electrolytes, such as difficulty in electrode wetting, low lithium-ion transference number, large concentration polarization, and poor long-term interface stability.

[0006] A second objective of this invention is to provide a method for preparing the aforementioned eutectic electrolyte.

[0007] The third objective of this invention is to provide an integrated solid-state negative electrode sheet that has low interfacial impedance, excellent electrolyte-electrode interface compatibility, and interface stability.

[0008] The fourth objective of this invention is to provide a solid-state battery.

[0009] In order to achieve the above-mentioned objectives of the present invention, the following technical solution is adopted: The present invention provides a eutectic electrolyte, wherein the raw materials of the eutectic electrolyte include: a eutectic precursor, a crosslinking agent, and an initiator; The eutectic precursor comprises a hydrogen donor, a hydrogen acceptor, and an amide-siloxane polymer monomer; the structural formula of the amide-siloxane polymer monomer is: R1, R2, and R3 are each independently any one of alkyl, alkoxy, and siloxy groups.

[0010] Furthermore, R1, R2 and R3 are each independently any one of methyl, propyl, ethoxy and trimethylsiloxy.

[0011] Furthermore, it includes at least one of the following features (1) to (4); (1) The hydrogen donor includes nitrile compounds; (2) The hydrogen acceptor includes a lithium salt; (3) The molar ratio of the hydrogen donor to the hydrogen acceptor is (3~6):1; (4) The mass of the amide siloxane polymer monomer accounts for 8% to 20% of the total mass of the eutectic precursor.

[0012] Furthermore, it includes at least one of the following features (1) to (4); (1) The crosslinking agent includes at least one of pentaerythritol tetraacrylate, polyethylene glycol dimethacrylate, polyethylene glycol diacrylate, di(trimethylolpropane)tetraacrylate and ethoxylated trimethylolpropane triacrylate; (2) The initiator includes a photoinitiator; (3) The mass ratio of the eutectic precursor to the crosslinking agent is (7~9):(1~3); (4) The mass of the initiator is 1% to 3% of the total mass of the eutectic precursor and the crosslinking agent.

[0013] The present invention also provides a method for preparing the eutectic electrolyte as described above, comprising the following steps: The raw materials for the eutectic electrolyte are mixed to obtain a eutectic electrolyte precursor solution; the eutectic electrolyte precursor solution is subjected to a polymerization reaction to obtain the eutectic electrolyte.

[0014] Further, the method for preparing the eutectic electrolyte precursor solution includes: mixing a hydrogen acceptor and a hydrogen donor under heating and stirring to obtain a first mixed solution; cooling the first mixed solution and adding an amide siloxane polymer monomer to obtain a second mixed solution; mixing the second mixed solution, a crosslinking agent, and an initiator to obtain the eutectic electrolyte precursor solution. And / or, the polymerization reaction includes ultraviolet light irradiation for 2 to 5 minutes.

[0015] The present invention also provides an integrated solid-state negative electrode sheet, comprising: a current collector and a negative electrode layer disposed on the surface of the current collector; the negative electrode layer comprises a negative electrode active material, a conductive agent, a binder, a eutectic electrolyte and an oxide solid electrolyte as described above.

[0016] Furthermore, the mass of the eutectic electrolyte is 5% to 15% of the total mass of the negative electrode active material, the conductive agent, the binder, and the oxide solid electrolyte.

[0017] The present invention also provides a solid-state battery, comprising the integrated solid-state negative electrode, positive electrode and solid-state electrolyte as described above.

[0018] Furthermore, the solid electrolyte is mainly obtained by thermal polymerization of acrylate monomers, lithium salts, plasticizers, crosslinking agents and thermal initiators.

[0019] Compared with the prior art, the beneficial effects of the present invention are as follows: The eutectic electrolyte of this invention uses hydrogen donors, hydrogen acceptors, and amide-siloxane polymer monomers as raw materials to form a polymer eutectic electrolyte. Through the structural design of the amide-siloxane polymer monomers, flexible siloxanes promote ion migration and inhibit electrode expansion. The eutectic relationship between the amide groups and lithium salt promotes the dissociation of lithium salt and endows the eutectic electrolyte with in-situ curing properties. By optimizing the interactions between the eutectic components, the strong coordination environment of lithium ions is decoupled, increasing lithium ion concentration, enhancing ion transference number, suppressing concentration polarization, inhibiting lithium dendrite growth, and improving ionic conductivity and ion transport performance. Simultaneously, it also exhibits excellent interfacial compatibility and long-term interfacial stability.

[0020] The integrated solid-state negative electrode of the present invention incorporates a eutectic electrolyte to fill the voids in the negative electrode, forming a high ion channel, which improves the interfacial contact between the electrolyte and the electrode and suppresses electrode expansion; optimizes the interfacial compatibility between the electrolyte and the electrode, and reduces interfacial impedance; effectively avoids the problem of poor electrode wetting caused by the high viscosity of the eutectic electrolyte; thereby improving the rate performance and cycle life of the solid-state battery. Attached Figure Description

[0021] To more clearly illustrate the technical solutions of the embodiments of the present invention, the accompanying drawings used in the embodiments will be briefly introduced below. It should be understood that the following drawings only show some embodiments of the present invention and should not be regarded as a limitation of the scope. For those skilled in the art, other related drawings can be obtained from these drawings without creative effort.

[0022] Figure 1The cycle capacity of the solid-state batteries of Embodiment 1, Embodiment 2, Comparative Example 1 and Comparative Example 3 of the present invention is shown.

[0023] Figure 2 The constant current ratio for cyclic charging in Embodiments 1, 2, 1, and 3 of the present invention is shown.

[0024] Figure 3 The above describes the rate charging tests of Embodiment 1, Embodiment 2, Comparative Example 1, and Comparative Example 3 of the present invention.

[0025] Figure 4 EIS tests were performed on Examples 1, 2, 1, and 3 of the present invention. Detailed Implementation

[0026] The technical solution of the present invention will be clearly and completely described below with reference to the accompanying drawings and specific embodiments. However, those skilled in the art will understand that the embodiments described below are some embodiments of the present invention, but not all embodiments, and are only used to illustrate the present invention, and should not be regarded as limiting the scope of the present invention. Based on the embodiments of the present invention, all other embodiments obtained by those skilled in the art without creative effort are within the scope of protection of the present invention. Where specific conditions are not specified in the embodiments, conventional conditions or conditions recommended by the manufacturer shall be followed. Where the manufacturers of reagents or instruments are not specified, they are all conventional products that can be purchased commercially.

[0027] In some embodiments of the present invention, a eutectic electrolyte is provided, wherein the raw materials of the eutectic electrolyte include: a eutectic precursor, a crosslinking agent, and an initiator; The eutectic precursor includes a hydrogen donor, a hydrogen acceptor, and an amide-siloxane polymer monomer; the structural formula of the amide-siloxane polymer monomer is: R1, R2, and R3 are each independently any one of alkyl, alkoxy, and siloxy groups.

[0028] The eutectic electrolyte of the present invention is a ternary eutectic electrolyte; it uses hydrogen donors, hydrogen acceptors and amide siloxane polymer monomers as raw materials to polymerize and form a polymer eutectic electrolyte.

[0029] Through the structural design of amide-siloxane polymer monomers, flexible siloxanes promote ion migration and suppress electrode expansion. The eutectic formation of amide groups and lithium salts promotes the dissociation of lithium salts and endows the eutectic electrolyte with in-situ curing properties.

[0030] By optimizing the interactions between eutectic components, the strong coordination environment of lithium ions is decoupled, increasing lithium ion concentration, enhancing ion transference number, suppressing concentration polarization, inhibiting lithium dendrite growth, and improving ionic conductivity and ion transport performance.

[0031] Eutectic electrolytes also exhibit excellent interfacial compatibility and long-term interfacial stability, improving the contact between the electrolyte and electrode interfaces and reducing interfacial impedance.

[0032] In some embodiments of the present invention, R1, R2 and R3 are each independently any one of methyl, propyl, ethoxy and trimethylsiloxy.

[0033] In some embodiments of the present invention, the method for preparing amide-siloxane polymer monomers includes: reacting aminosiloxane, organic amine, polymerization inhibitor and methacryloyl chloride in a solvent to obtain amide-siloxane polymer monomers.

[0034] In some embodiments of the present invention, the method for preparing amide-siloxane polymer monomers includes the following steps: Under a nitrogen atmosphere, aminosiloxane, organic amine, polymerization inhibitor and solvent are mixed to obtain a mixed solution; a solution containing methacryloyl chloride is added dropwise to the above mixed solution, and the mixture is stirred in an ice bath for 0.5-1.5 h, then stirred at room temperature for 2-4 h; then, after quenching with water, extraction and washing, drying and filtration, rotary evaporation and column chromatography purification, the amide siloxane polymer monomer is obtained. The structural formula of aminosiloxane is as follows: R1, R2 and R3 are each independently one of alkyl, alkoxy and siloxy; preferably, R1, R2 and R3 are each independently one of methyl, propyl, ethoxy and trimethylsiloxy.

[0035] In some embodiments of the present invention, the aminosiloxane includes any one of 3-aminopropyltriethoxysilane, γ-aminopropylmethyldiethoxysilane, and 3-aminopropylbis(trimethylsiloxy)methylsilane.

[0036] In some embodiments of the present invention, the molar ratio of methacryloyl chloride to aminosiloxane is (1~1.3):1.

[0037] In some embodiments of the present invention, organic amines include, but are not limited to, triethylamine (TEA).

[0038] In some embodiments of the present invention, the polymerization inhibitor includes at least one of 4-methoxyphenol, hydroquinone, and p-tert-butylcatechol.

[0039] In some embodiments of the present invention, the solvent includes, but is not limited to, dichloromethane; the solvent in the solution containing methacryloyl chloride includes, but is not limited to, dichloromethane.

[0040] In some embodiments of the present invention, the hydrogen donor includes nitrile compounds; preferably, the nitrile compounds include succinic anionyl nitrile and its derivatives.

[0041] In some embodiments of the present invention, the hydrogen acceptor includes a lithium salt; preferably, the lithium salt includes at least one of LiPF6, LiBF4, LiPOF2, LiTFSI, LiFSI, LiODFB and LiClO4.

[0042] In some embodiments of the invention, the molar ratio of hydrogen donor to hydrogen acceptor is (3 to 6):1; typically, but not limitingly, for example, the molar ratio of hydrogen donor to hydrogen acceptor can be 3:1, 4:1, 5:1, 6:1, and any value between any two of these.

[0043] In some embodiments of the invention, the mass of the amide-siloxane polymer monomer accounts for 8% to 20% of the total mass of the eutectic precursor; typically, but not limitingly, for example, the mass of the amide-siloxane polymer monomer accounts for 8%, 10%, 12%, 14%, 16%, 18%, 20% of the total mass of the eutectic precursor, and any value between any two thereof.

[0044] In some embodiments of the present invention, the crosslinking agent includes at least one of pentaerythritol tetraacrylate, polyethylene glycol dimethacrylate, polyethylene glycol diacrylate, di(trimethylolpropane)tetraacrylate, and ethoxylated trimethylolpropane triacrylate.

[0045] In some embodiments of the present invention, the initiator includes a photoinitiator; preferably, the photoinitiator includes at least one selected from benzoin methyl ether, benzoin ethyl ether, and 2-hydroxy-2-methyl-1-phenyl-1-propanone.

[0046] In some embodiments of the present invention, the mass ratio of the eutectic precursor to the crosslinking agent is (7~9):(1~3); typically, but not limitingly, for example, the mass ratio of the eutectic precursor to the crosslinking agent can be 9:1, 8:2, 7:3, and any value between any two of these.

[0047] In some embodiments of the invention, the mass of the initiator is 1% to 3% of the total mass of the eutectic precursor and the crosslinking agent; typically, but not limitingly, for example, the mass of the initiator is 1%, 2%, 3% of the total mass of the eutectic precursor and the crosslinking agent, and any value between any two thereof.

[0048] In some embodiments of the present invention, a method for preparing the above-mentioned eutectic electrolyte is also provided, comprising the following steps: The raw materials for the eutectic electrolyte are mixed to obtain a eutectic electrolyte precursor solution; the eutectic electrolyte precursor solution undergoes a polymerization reaction to obtain the eutectic electrolyte.

[0049] In some embodiments of the present invention, the method for preparing the eutectic electrolyte precursor solution includes: mixing a hydrogen acceptor and a hydrogen donor under heating and stirring to obtain a first mixed solution; cooling the first mixed solution and adding an amide siloxane polymer monomer and mixing to obtain a second mixed solution; mixing the second mixed solution, a crosslinking agent, and an initiator to obtain the eutectic electrolyte precursor solution; preferably, heating the solid hydrogen donor to a liquid state, then adding the hydrogen acceptor, heating and stirring to obtain the first mixed solution; the heating and stirring temperature is 40~70℃ (e.g., 40℃, 50℃, 60℃, 70℃, etc.), and the time is 1~3h (e.g., 1h, 2h, 3h, etc.); cooling to room temperature (e.g., 25℃); mixing includes: stirring at 20~30℃ (e.g., 25℃) for 1~3h (e.g., 1h, 2h, 3h, etc.).

[0050] In some embodiments of the present invention, the polymerization reaction includes irradiation with ultraviolet light for 2 to 5 minutes; typically, but not limitingly, for example, the polymerization reaction time can be 2 minutes, 3 minutes, 4 minutes, 5 minutes, and any value between any two thereof; preferably, the polymerization reaction includes irradiation with an ultraviolet lamp with a wavelength of 356 nm and a power of 80 W for 2 to 5 minutes.

[0051] In some embodiments of the present invention, an integrated solid-state negative electrode sheet is also provided, comprising: a current collector and a negative electrode layer disposed on the surface of the current collector; the negative electrode layer comprises a negative electrode active material, a conductive agent, a binder, the aforementioned eutectic electrolyte and an oxide solid electrolyte.

[0052] The integrated solid-state negative electrode of the present invention incorporates a eutectic electrolyte to fill the voids in the negative electrode, forming a high ion channel. This improves the interface contact and polymerization uniformity between the electrolyte and the electrode, and inhibits electrode expansion. It effectively avoids the problem of poor electrode wetting caused by the high viscosity of the eutectic electrolyte.

[0053] The integrated solid-state negative electrode of the present invention does not rely on the traditional impregnation process, optimizes the interfacial compatibility between the electrolyte and the electrode, reduces interfacial impedance, and improves the long-term stability of the interface.

[0054] This invention constructs an integrated solid-state anode by using a eutectic electrolyte, an oxide solid electrolyte, and an anode active material, thereby improving ionic conductivity, ion transport, interfacial compatibility, and interfacial stability.

[0055] In some embodiments of the present invention, the mass of the eutectic electrolyte is 5% to 15% of the total mass of the negative electrode active material, conductive agent, binder and oxide solid electrolyte; typically, but not limitingly, for example, the mass of the eutectic electrolyte is 5%, 6%, 7%, 8%, 9%, 10%, 11%, 12%, 13%, 14%, 15% of the total mass of the negative electrode active material, conductive agent, binder and oxide solid electrolyte and any value between any two of these.

[0056] In some embodiments of the present invention, the negative electrode active material includes at least one of graphite, soft carbon, hard carbon, silicon-carbon materials, and silicon-oxygen materials.

[0057] In some embodiments of the present invention, the conductive agent includes at least one of SP, acetylene black, Ketjen black and CNT.

[0058] In some embodiments of the present invention, the adhesive includes an oil-based adhesive and / or a water-based adhesive; preferably, the oil-based adhesive includes PVDF, and the water-based adhesive includes at least one of PAA, CMC, and SBR.

[0059] In some embodiments of the present invention, the oxide solid electrolyte includes at least one of LLNOF, LLTO and LLZO.

[0060] In some embodiments of the present invention, the mass ratio of the negative electrode active material, conductive agent, binder and oxide solid electrolyte is 93~95:0.3~1.5:1.5~2:2~4.

[0061] In some embodiments of the present invention, the current collector includes, but is not limited to, a copper current collector.

[0062] In some embodiments of the present invention, a method for preparing the above-mentioned integrated solid-state negative electrode is also provided, comprising the following steps: A negative electrode active material, conductive agent, binder, eutectic electrolyte precursor solution, and oxide solid electrolyte are dispersed in an organic solvent to obtain a negative electrode slurry. The negative electrode slurry is coated onto a fluid, and polymerization, drying, and rolling are carried out sequentially to obtain an integrated solid negative electrode sheet. Preferably, the polymerization reaction includes ultraviolet light irradiation for 2-5 minutes; for example, irradiation under an ultraviolet lamp with a wavelength of 356 nm and a power of 80 W for 2-5 minutes. Drying includes drying to remove the solvent, for example, drying at 90°C for 3 hours. The organic solvent includes, but is not limited to, NMP.

[0063] In some embodiments of the present invention, a solid-state battery is also provided, including the above-described integrated solid-state negative electrode, positive electrode and solid electrolyte.

[0064] Solid-state batteries using the integrated solid-state negative electrode of this invention exhibit excellent rate performance and cycle life.

[0065] In some embodiments of the present invention, the solid electrolyte is mainly obtained by thermal polymerization of acrylate monomers, lithium salts, plasticizers, crosslinking agents and thermal initiators.

[0066] In some embodiments of the present invention, the method for preparing a solid electrolyte includes: mixing an acrylate monomer, a lithium salt, a plasticizer, and a crosslinking agent to obtain a mixed solution; adding a thermal initiator to the mixed solution to obtain a solid electrolyte precursor; and thermally polymerizing the solid electrolyte precursor to obtain a solid electrolyte.

[0067] In some embodiments of the present invention, the acrylate monomers include at least one of butyl acrylate, methacrylate, isooctyl acrylate, trifluoroethyl acrylate, and hexafluorobutyl acrylate.

[0068] In some embodiments of the present invention, the lithium salt is at least one selected from LiPF6, LiBF4, LiPOF2, LiTFSI, LiFSI, LiODFB, LiClO4, and LiNO3.

[0069] In some embodiments of the present invention, in the method for preparing the solid electrolyte, the concentration of lithium salt in the mixed solution is 0.5 to 1.5 mol / L; typically, but not limitingly, for example, the concentration of lithium salt in the mixed solution can be 0.5 mol / L, 1 mol / L, 1.5 mol / L, and any value between any two thereof.

[0070] In some embodiments of the present invention, the plasticizer includes succinic acid and / or fluoroethylene carbonate.

[0071] In some embodiments of the present invention, the crosslinking agent includes at least one of pentaerythritol tetraacrylate, polyethylene glycol dimethacrylate, polyethylene glycol diacrylate, di(trimethylolpropane)tetraacrylate, and ethoxylated trimethylolpropane triacrylate.

[0072] In some embodiments of the invention, the mass ratio of acrylate monomers, plasticizers and crosslinking agents is (5~8):(1~4):1; typically, but not limitingly, for example, the mass ratio of acrylate monomers, plasticizers and crosslinking agents is 5:4:1, 6:3:1, 7:2:1, 8:1:1 and any value between any two of these.

[0073] In some embodiments of the present invention, the thermal initiator includes, but is not limited to, AIBN.

[0074] In some embodiments of the present invention, in the method for preparing the solid electrolyte, the mass of AIBN is 0.05% to 2% of the total mass of the mixed solution; typically, but not limitingly, for example, the mass of AIBN is 0.05%, 0.1%, 0.5%, 1%, 1.5%, 2% of the total mass of the mixed solution, and any value between any two thereof.

[0075] In some embodiments of the present invention, the temperature of thermal polymerization is 40~70°C and the time is 1~48h; typically, but not limitingly, for example, the temperature of thermal polymerization can be 40°C, 50°C, 60°C, 70°C and any value between any two thereof; the time can be 1h, 5h, 10h, 15h, 20h, 25h, 30h, 35h, 40h, 48h and any value between any two thereof.

[0076] In some embodiments of the present invention, the positive electrode includes, but is not limited to, the NCM811 electrode.

[0077] In some embodiments of the present invention, the solid-state battery further includes a separator; the separator includes, but is not limited to, a PE separator.

[0078] In some embodiments of the present invention, a method for preparing the above-mentioned solid-state battery is also provided, comprising the following steps: A solid electrolyte precursor is injected into a solid cell, and after standing, it undergoes thermal polymerization to obtain a solid battery. The solid cell includes an integrated solid negative electrode, a positive electrode, and a separator. Preferably, the standing time is 20-30 hours (e.g., 20 hours, 22 hours, 24 hours, 26 hours, 28 hours, 30 hours, etc.); the thermal polymerization temperature is 40-70°C (e.g., 40°C, 50°C, 60°C, 70°C, etc.), and the time is 1-48 hours (e.g., 1 hour, 5 hours, 10 hours, 15 hours, 20 hours, 25 hours, 30 hours, 35 hours, 40 hours, 48 ​​hours, etc.).

[0079] Example 1 The method for preparing the integrated solid-state negative electrode provided in this embodiment includes the following steps: 11.72 g of succinate was heated and stirred at 50 °C until it became liquid. Then, 5.48 g of LiFSI was added, and the mixture was stirred at 50 °C for 1 h to obtain a first mixed solution. The first mixed solution was cooled to 25 °C, and 2.8 g of amide siloxane polymer monomer was added. The mixture was stirred at 25 °C for 2 h to obtain a second mixed solution. The second mixed solution and crosslinking agent (di(trimethylolpropane)tetraacrylate) were mixed at a mass ratio of 4:1, and then a photoinitiator (2-hydroxy-2-methyl-1-phenyl-1-propanone) was added. The mass of the photoinitiator was 2% of the total mass of the second mixed solution and the crosslinking agent to obtain a eutectic electrolyte precursor solution. Graphite, silicon carbide, CNTs, PVDF, and LLNOF were mixed in NMP at a mass ratio of 85.4:9.4:0.5:1.7:3. A eutectic electrolyte precursor solution, comprising 10% of the total mass of graphite, silicon carbide, CNTs, PVDF, and LLNOF, was then added and mixed to obtain a negative electrode slurry. This slurry was coated onto a copper current collector, irradiated for 3 minutes under an 80W UV lamp at a wavelength of 356 nm, dried at 90°C for 3 hours, and then rolled to a compaction density of 1.6 g / cm³. 3 This yields an integrated solid-state negative electrode.

[0080] The solid-state battery preparation method provided in this embodiment includes the following steps: Isooctyl acrylate, trifluoroethyl acrylate, succinate, and di(trimethylolpropane)tetraacrylate were mixed in a mass ratio of 3:2:4:1, and then LiFSI was added to obtain a mixed solution with a LiFSI concentration of 1.2 mol / L. AIBN was then added to the mixed solution at a mass of 0.15% of the mixed solution mass to obtain a solid electrolyte precursor. A solid electrolyte precursor is injected into a solid cell, which includes an NCM811 positive electrode, a PE separator, and the aforementioned integrated solid negative electrode. The cell has an N / P ratio of 1.15 and a designed capacity of 0.08 Ah. The cell is then left to stand for 24 hours and polymerized at 60°C for 2 hours to obtain a solid-state battery.

[0081] The preparation method of the amide-siloxane polymer monomer in this embodiment includes the following steps: Under a nitrogen atmosphere, 10 g of 3-aminopropylbis(trimethylsiloxy)methylsilane was dissolved in 160 mL of anhydrous dichloromethane, and then 3.6 g of TEA and 0.01 g of 4-methoxyphenol were added. After stirring, a mixed solution was obtained. 3.54 g of methacryloyl chloride was diluted in 10 mL of anhydrous dichloromethane and slowly added dropwise to the above mixed solution. The mixture was stirred for 1 h in an ice bath and then stirred for 3 h at room temperature (25 °C). After quenching with water, extraction and washing, drying and filtration, rotary evaporation and column chromatography purification were performed to obtain the amide siloxane polymer monomer. The structural formula of 3-aminopropylbis(trimethylsiloxy)methylsilane is: The structural formula of the amide-siloxane polymer monomer is: .

[0082] Example 2 The method for preparing the integrated solid-state negative electrode provided in this embodiment includes the following steps: 10.13 g of succinate was heated and stirred at 50 °C until it became liquid. Then, 7.87 g of LiFSI was added, and the mixture was stirred at 50 °C for 1 h to obtain a first mixed solution. The first mixed solution was cooled to 25 °C, and 2 g of amide siloxane polymer monomer (same as in Example 1) was added. The mixture was stirred at 25 °C for 2 h to obtain a second mixed solution. The second mixed solution and crosslinking agent (di(trimethylolpropane)tetraacrylate) were mixed at a mass ratio of 4:1, and then a photoinitiator (2-hydroxy-2-methyl-1-phenyl-1-propanone) was added. The mass of the photoinitiator was 2% of the total mass of the second mixed solution and the crosslinking agent to obtain a eutectic electrolyte precursor solution. Graphite, silicon carbide, CNTs, PVDF, and LLNOF were mixed in NMP at a mass ratio of 85.4:9.4:0.5:1.7:3. A eutectic electrolyte precursor solution, comprising 10% of the total mass of graphite, silicon carbide, CNTs, PVDF, and LLNOF, was then added and mixed to obtain a negative electrode slurry. This slurry was coated onto a copper current collector, irradiated for 3 minutes under an 80W UV lamp at a wavelength of 356 nm, dried at 90°C for 3 hours, and then rolled to a compaction density of 1.6 g / cm³. 3 This yields an integrated solid-state negative electrode.

[0083] The solid-state battery preparation method provided in this embodiment includes the following steps: Isooctyl acrylate, trifluoroethyl acrylate, succinate, and di(trimethylolpropane)tetraacrylate were mixed in a mass ratio of 3:2:4:1, and then LiFSI was added to obtain a mixed solution with a LiFSI concentration of 1.2 mol / L. AIBN was then added to the mixed solution at a mass of 0.15% of the mixed solution mass to obtain a solid electrolyte precursor. A solid electrolyte precursor is injected into a solid cell, which includes an NCM811 positive electrode, a PE separator, and the aforementioned integrated solid negative electrode. The cell has an N / P ratio of 1.15 and a designed capacity of 0.08 Ah. The cell is then left to stand for 24 hours and polymerized at 60°C for 2 hours to obtain a solid-state battery.

[0084] Example 3 The method for preparing the integrated solid-state negative electrode provided in this embodiment includes the following steps: 10.86 g of succinate was heated and stirred at 50 °C until it became liquid. Then, 6.34 g of LiFSI was added, and the mixture was stirred at 50 °C for 1 h to obtain a first mixed solution. The first mixed solution was cooled to 25 °C, and 2.8 g of amide siloxane polymer monomer was added. The mixture was stirred at 25 °C for 2 h to obtain a second mixed solution. The second mixed solution and crosslinking agent (di(trimethylolpropane)tetraacrylate) were mixed at a mass ratio of 9:1, and then a photoinitiator (2-hydroxy-2-methyl-1-phenyl-1-propanone) was added. The mass of the photoinitiator was 2% of the total mass of the second mixed solution and the crosslinking agent to obtain a eutectic electrolyte precursor solution. Graphite, silicon carbide, CNTs, PVDF, and LLZO were mixed in NMP at a mass ratio of 85.4:9.4:0.5:1.7:3. A eutectic electrolyte precursor solution, comprising 12% of the total mass of graphite, silicon carbide, CNTs, PVDF, and LLZO, was then added and mixed to obtain a negative electrode slurry. This slurry was coated onto a copper current collector, irradiated for 3 minutes under an 80W UV lamp at a wavelength of 356 nm, dried at 90°C for 3 hours, and then rolled to a compaction density of 1.6 g / cm³. 3 This yields an integrated solid-state negative electrode.

[0085] The solid-state battery preparation method provided in this embodiment includes the following steps: Isooctyl acrylate, trifluoroethyl acrylate, succinate, and di(trimethylolpropane)tetraacrylate were mixed in a mass ratio of 3:2:4:1, and then LiFSI was added to obtain a mixed solution with a LiFSI concentration of 1.2 mol / L. AIBN was then added to the mixed solution at a mass of 0.15% of the mixed solution mass to obtain a solid electrolyte precursor. A solid electrolyte precursor is injected into a solid cell, which includes an NCM811 positive electrode, a PE separator, and the aforementioned integrated solid negative electrode. The cell has an N / P ratio of 1.15 and a designed capacity of 0.08 Ah. The cell is then left to stand for 24 hours and polymerized at 60°C for 2 hours to obtain a solid-state battery.

[0086] The preparation method of the amide-siloxane polymer monomer in this embodiment includes the following steps: Under a nitrogen atmosphere, 10 g of γ-aminopropylmethyldiethoxysilane was dissolved in 130 mL of anhydrous dichloromethane, and then 5.31 g of TEA and 0.01 g of 4-methoxyphenol were added. After stirring, a mixed solution was obtained. 5.18 g of methacryloyl chloride was diluted in 10 mL of anhydrous dichloromethane and slowly added dropwise to the above mixed solution. The mixture was stirred for 1 h in an ice bath and then stirred for 3 h at room temperature (25 °C). After quenching with water, extraction and washing, drying and filtration, rotary evaporation and column chromatography purification were performed to obtain the amide siloxane polymer monomer. The structural formula of γ-aminopropylmethyldiethoxysilane is: The structural formula of the amide-siloxane polymer monomer is: .

[0087] Example 4 The method for preparing the integrated solid-state negative electrode provided in this embodiment includes the following steps: 12.27 g of succinate was heated and stirred at 50 °C until it became liquid. Then, 5.73 g of LiFSI was added, and the mixture was stirred at 50 °C for 1 h to obtain a first mixed solution. The first mixed solution was cooled to 25 °C, and 2 g of amide siloxane polymer monomer (same as in Example 3) was added. The mixture was stirred at 25 °C for 2 h to obtain a second mixed solution. The second mixed solution and crosslinking agent (di(trimethylolpropane)tetraacrylate) were mixed at a mass ratio of 4:1, and then a photoinitiator (2-hydroxy-2-methyl-1-phenyl-1-propanone) was added. The mass of the photoinitiator was 2% of the total mass of the second mixed solution and the crosslinking agent to obtain a eutectic electrolyte precursor solution. Graphite, silicon carbide, CNTs, PVDF, and LLNOF were mixed in NMP at a mass ratio of 85.4:9.4:0.5:1.7:3. A eutectic electrolyte precursor solution, comprising 10% of the total mass of graphite, silicon carbide, CNTs, PVDF, and LLNOF, was then added and mixed to obtain a negative electrode slurry. This slurry was coated onto a copper current collector, irradiated for 3 minutes under an 80W UV lamp at a wavelength of 356 nm, dried at 90°C for 3 hours, and then rolled to a compaction density of 1.6 g / cm³. 3 This yields an integrated solid-state negative electrode.

[0088] The solid-state battery preparation method provided in this embodiment includes the following steps: Isooctyl acrylate, trifluoroethyl acrylate, succinate, and di(trimethylolpropane)tetraacrylate were mixed in a mass ratio of 3:2:4:1, and then LiFSI was added to obtain a mixed solution with a LiFSI concentration of 1.2 mol / L. AIBN was then added to the mixed solution at a mass of 0.15% of the mixed solution mass to obtain a solid electrolyte precursor. A solid electrolyte precursor is injected into a solid cell, which includes an NCM811 positive electrode, a PE separator, and the aforementioned integrated solid negative electrode. The cell has an N / P ratio of 1.15 and a designed capacity of 0.08 Ah. The cell is then left to stand for 24 hours and polymerized at 60°C for 2 hours to obtain a solid-state battery.

[0089] Example 5 The method for preparing the integrated solid-state negative electrode provided in this embodiment includes the following steps: 11.72 g of succinate was heated and stirred at 50 °C until it became liquid. Then, 5.48 g of LiFSI was added, and the mixture was stirred at 50 °C for 1 h to obtain a first mixed solution. The first mixed solution was cooled to 25 °C, and 2.8 g of amide siloxane polymer monomer was added. The mixture was stirred at 25 °C for 2 h to obtain a second mixed solution. The second mixed solution and crosslinking agent (di(trimethylolpropane)tetraacrylate) were mixed at a mass ratio of 9:1. Then, a photoinitiator (2-hydroxy-2-methyl-1-phenyl-1-propanone) was added. The mass of the photoinitiator was 2% of the total mass of the second mixed solution and the crosslinking agent to obtain a eutectic electrolyte precursor solution. Graphite, silicon carbide, CNTs, PVDF, and LLNOF were mixed in NMP at a mass ratio of 85.4:9.4:0.5:1.7:3. A eutectic electrolyte precursor solution, comprising 10% of the total mass of graphite, silicon carbide, CNTs, PVDF, and LLNOF, was then added and mixed to obtain a negative electrode slurry. This slurry was coated onto a copper current collector, irradiated for 3 minutes under an 80W UV lamp at a wavelength of 356 nm, dried at 90°C for 3 hours, and then rolled to a compaction density of 1.6 g / cm³. 3 This yields an integrated solid-state negative electrode.

[0090] The solid-state battery preparation method provided in this embodiment includes the following steps: The following mixtures were prepared by mixing isooctyl acrylate, hexafluorobutyl acrylate, succinate, and di(trimethylolpropane)tetraacrylate in a mass ratio of 3:2:4:1, and then LiFSI was added to obtain a mixed solution with a LiFSI concentration of 1.2 mol / L. AIBN was then added to the mixed solution at a mass of 0.15% of the mixed solution mass to obtain a solid electrolyte precursor. A solid electrolyte precursor is injected into a solid cell, which includes an NCM811 positive electrode, a PE separator, and the aforementioned integrated solid negative electrode. The cell has an N / P ratio of 1.15 and a designed capacity of 0.08 Ah. The cell is then left to stand for 24 hours and polymerized at 60°C for 2 hours to obtain a solid-state battery.

[0091] The preparation method of the amide-siloxane polymer monomer in this embodiment includes the following steps: Under a nitrogen atmosphere, 10 g of 3-aminopropyltriethoxysilane was dissolved in 130 mL of anhydrous dichloromethane, and then 4.4 g of TEA and 0.01 g of 4-methoxyphenol were added. After stirring, a mixed solution was obtained. 4.28 g of methacryloyl chloride was diluted in 10 mL of anhydrous dichloromethane and slowly added dropwise to the above mixed solution. The mixture was stirred for 1 h in an ice bath and then stirred for 3 h at room temperature (25 °C). After quenching with water, extraction and washing, drying and filtration, rotary evaporation and column chromatography purification were performed to obtain the amide siloxane polymer monomer. The structural formula of 3-aminopropyltriethoxysilane is: The structural formula of the amide-siloxane polymer monomer is: .

[0092] Example 6 The method for preparing the integrated solid-state negative electrode provided in this embodiment includes the following steps: 10.02 g of succinate was heated and stirred at 50 °C until it became liquid. Then, 7.18 g of LiTFSI was added, and the mixture was stirred at 50 °C for 1 h to obtain a first mixed solution. The first mixed solution was cooled to 25 °C, and 2.8 g of amide siloxane polymer monomer (same as in Example 5) was added. The mixture was stirred at 25 °C for 2 h to obtain a second mixed solution. The second mixed solution and crosslinking agent (di(trimethylolpropane)tetraacrylate) were mixed at a mass ratio of 9:1, and then a photoinitiator (2-hydroxy-2-methyl-1-phenyl-1-propanone) was added. The mass of the photoinitiator was 2% of the total mass of the second mixed solution and the crosslinking agent to obtain a eutectic electrolyte precursor solution. Graphite, silicon carbide, CNTs, PVDF, and LLZO were mixed in NMP at a mass ratio of 85.4:9.4:0.5:1.7:3. A eutectic electrolyte precursor solution, comprising 10% of the total mass of graphite, silicon carbide, CNTs, PVDF, and LLZO, was then added and mixed to obtain a negative electrode slurry. This slurry was coated onto a copper current collector, irradiated for 3 minutes under an 80W UV lamp at a wavelength of 356 nm, dried at 90°C for 3 hours, and then rolled to a compaction density of 1.6 g / cm³. 3 This yields an integrated solid-state negative electrode.

[0093] The solid-state battery preparation method provided in this embodiment includes the following steps: The isooctyl acrylate, trifluoroethyl acrylate, succinate, and pentaerythritol tetraacrylate were mixed in a mass ratio of 3:2:4:1, and then LiTFSI was added to obtain a mixed solution with a concentration of 1.2 mol / L. AIBN was then added to the mixed solution at a mass of 0.15% of the mass of the mixed solution to obtain a solid electrolyte precursor. A solid electrolyte precursor is injected into a solid cell, which includes an NCM811 positive electrode, a PE separator, and the aforementioned integrated solid negative electrode. The cell has an N / P ratio of 1.15 and a designed capacity of 0.08 Ah. The cell is then left to stand for 24 hours and polymerized at 60°C for 2 hours to obtain a solid-state battery.

[0094] Comparative Example 1 The method for preparing the integrated solid-state negative electrode provided in this comparative example includes the following steps: 13.63 g of succinate was heated and stirred at 50 °C until it became liquid. Then, 6.37 g of LiFSI was added and stirred at 50 °C for 1 h to obtain a mixed solution. The mixed solution and crosslinking agent (di(trimethylolpropane)tetraacrylate) were mixed at a mass ratio of 4:1. Then, a photoinitiator (2-hydroxy-2-methyl-1-phenyl-1-propanone) was added. The mass of the photoinitiator was 2% of the total mass of the mixed solution and the crosslinking agent to obtain a eutectic electrolyte precursor solution. Graphite, silicon carbide, CNTs, PVDF, and LLNOF were mixed in NMP at a mass ratio of 85.4:9.4:0.5:1.7:3. A eutectic electrolyte precursor solution, comprising 10% of the total mass of graphite, silicon carbide, CNTs, PVDF, and LLNOF, was then added and mixed to obtain a negative electrode slurry. This slurry was coated onto a copper current collector, irradiated for 3 minutes under an 80W UV lamp at a wavelength of 356 nm, dried at 90°C for 3 hours, and then rolled to a compaction density of 1.6 g / cm³. 3 This yields an integrated solid-state negative electrode.

[0095] The solid-state battery preparation method provided in this comparative example includes the following steps: Isooctyl acrylate, trifluoroethyl acrylate, succinate, and di(trimethylolpropane)tetraacrylate were mixed in a mass ratio of 3:2:4:1, and then LiFSI was added to obtain a mixed solution with a LiFSI concentration of 1.2 mol / L. AIBN was then added to the mixed solution at a mass of 0.15% of the mixed solution mass to obtain a solid electrolyte precursor. A solid electrolyte precursor is injected into a solid cell, which includes an NCM811 positive electrode, a PE separator, and the aforementioned integrated solid negative electrode. The cell has an N / P ratio of 1.15 and a designed capacity of 0.08 Ah. The cell is then left to stand for 24 hours and polymerized at 60°C for 2 hours to obtain a solid-state battery.

[0096] Comparative Example 2 The method for preparing the integrated solid-state negative electrode provided in this comparative example includes the following steps: 15.03 g of amide-siloxane polymer monomer (same as in Example 1) and 4.97 g of LiFSI were stirred at 25 °C for 1 h to obtain a mixed solution; the mixed solution and crosslinking agent (di(trimethylolpropane)tetraacrylate) were mixed at a mass ratio of 4:1, and then a photoinitiator (2-hydroxy-2-methyl-1-phenyl-1-propanone) was added, the mass of which was 2% of the total mass of the mixed solution and the crosslinking agent, to obtain a eutectic electrolyte precursor solution; Graphite, silicon carbide, CNTs, PVDF, and LLNOF were mixed in NMP at a mass ratio of 85.4:9.4:0.5:1.7:3. A eutectic electrolyte precursor solution, comprising 10% of the total mass of graphite, silicon carbide, CNTs, PVDF, and LLNOF, was then added and mixed to obtain a negative electrode slurry. This slurry was coated onto a copper current collector, irradiated for 3 minutes under an 80W UV lamp at a wavelength of 356 nm, dried at 90°C for 3 hours, and then rolled to a compaction density of 1.6 g / cm³. 3 This yields an integrated solid-state negative electrode.

[0097] The solid-state battery preparation method provided in this comparative example includes the following steps: Isooctyl acrylate, trifluoroethyl acrylate, succinate, and di(trimethylolpropane)tetraacrylate were mixed in a mass ratio of 3:2:4:1, and then LiFSI was added to obtain a mixed solution with a LiFSI concentration of 1.2 mol / L. AIBN was then added to the mixed solution at a mass of 0.15% of the mixed solution mass to obtain a solid electrolyte precursor. A solid electrolyte precursor is injected into a solid cell, which includes an NCM811 positive electrode, a PE separator, and the aforementioned integrated solid negative electrode. The cell has an N / P ratio of 1.15 and a designed capacity of 0.08 Ah. The cell is then left to stand for 24 hours and polymerized at 60°C for 2 hours to obtain a solid-state battery.

[0098] Comparative Example 3 The method for preparing the negative electrode sheet provided in this comparative example includes the following steps: Graphite, silicon carbide, CNTs, PVDF, and LLNOF were mixed in NMP at a mass ratio of 85.4:9.4:0.5:1.7:3 to obtain a negative electrode slurry. The negative electrode slurry was coated onto a copper current collector, dried at 90°C for 3 hours, and then rolled to a compaction density of 1.6 g / cm³. 3 This yields the negative electrode.

[0099] The solid-state battery preparation method provided in this comparative example includes the following steps: Isooctyl acrylate, trifluoroethyl acrylate, succinate, and di(trimethylolpropane)tetraacrylate were mixed in a mass ratio of 3:2:4:1, and then LiFSI was added to obtain a mixed solution with a LiFSI concentration of 1.2 mol / L. AIBN was then added to the mixed solution at a mass of 0.15% of the mixed solution mass to obtain a solid electrolyte precursor. A solid electrolyte precursor is injected into a solid cell, which includes an NCM811 positive electrode, a PE separator, and the aforementioned negative electrode. The cell has an N / P ratio of 1.15 and a designed capacity of 0.08 Ah. The cell is then left to stand for 24 hours and polymerized at 60°C for 2 hours to obtain a solid-state battery.

[0100] Test case The performance of the solid-state batteries prepared in Examples 1-6 and Comparative Examples 1-3 was tested, and the results are shown in Table 1; wherein, the cycle capacity of the solid-state batteries of Examples 1, 2, 1, and 3 is as follows: Figure 1 As shown, constant current during cyclic charging, for example Figure 2 As shown, the rate charging test is as follows: Figure 3 As shown, the EIS test is as follows Figure 4 As shown.

[0101] Cyclic performance test: conditions are: 25℃, 0.5C charge / discharge rate; test voltage range: 2.75~4.2V, constant current and constant voltage charge, constant current discharge.

[0102] Rate performance test: conditions: 25℃; rate: 0.2 / 0.33 / 0.5 / 1 / 2 / 3 / 0.2C (rate charging); test voltage range: 2.75~4.2V.

[0103] EIS test conditions: 25℃; frequency: 0.01~10kHz; amplitude: 5mV.

[0104] Table 1

[0105] From Table 1, Figure 1 , Figure 2 , Figure 3 and Figure 4 The electrical performance data show that the eutectic electrolyte of the present invention has high ionic conductivity and ion transport, and through the integrated electrolyte negative electrode technology, the compatibility of the electrolyte and electrode interface is optimized and the interface impedance is reduced, thereby improving the rate and cycle performance of the solid-state battery.

[0106] Although the present invention has been illustrated and described with specific embodiments, it should be understood that the above embodiments are only used to illustrate the technical solutions of the present invention, and not to limit them; those skilled in the art should understand that modifications can be made to the technical solutions described in the foregoing embodiments, or equivalent substitutions can be made to some or all of the technical features therein, without departing from the spirit and scope of the present invention; and these modifications or substitutions do not cause the essence of the corresponding technical solutions to deviate from the scope of the technical solutions of the embodiments of the present invention; therefore, this means that all such substitutions and modifications that fall within the scope of the present invention are included in the appended claims.

Claims

1. A eutectic electrolyte, characterized in that, The raw materials for the eutectic electrolyte include: eutectic precursor, crosslinking agent and initiator; The eutectic precursor comprises a hydrogen donor, a hydrogen acceptor, and an amide-siloxane polymer monomer; the structural formula of the amide-siloxane polymer monomer is: R1, R2, and R3 are each independently any one of alkyl, alkoxy, and siloxy groups.

2. The eutectic electrolyte according to claim 1, characterized in that, R1, R2 and R3 are each independently one of methyl, propyl, ethoxy and trimethylsiloxy.

3. The eutectic electrolyte according to claim 1, characterized in that, Includes at least one of the following features (1) to (4); (1) The hydrogen donor includes nitrile compounds; (2) The hydrogen acceptor includes a lithium salt; (3) The molar ratio of the hydrogen donor to the hydrogen acceptor is (3~6):1; (4) The mass of the amide siloxane polymer monomer accounts for 8% to 20% of the total mass of the eutectic precursor.

4. The eutectic electrolyte according to claim 1, characterized in that, Includes at least one of the following features (1) to (4); (1) The crosslinking agent includes at least one of pentaerythritol tetraacrylate, polyethylene glycol dimethacrylate, polyethylene glycol diacrylate, di(trimethylolpropane)tetraacrylate and ethoxylated trimethylolpropane triacrylate; (2) The initiator includes a photoinitiator; (3) The mass ratio of the eutectic precursor to the crosslinking agent is (7~9):(1~3); (4) The mass of the initiator is 1% to 3% of the total mass of the eutectic precursor and the crosslinking agent.

5. The method for preparing the eutectic electrolyte according to any one of claims 1 to 4, characterized in that, Includes the following steps: The raw materials for the eutectic electrolyte are mixed to obtain a eutectic electrolyte precursor solution; the eutectic electrolyte precursor solution is subjected to a polymerization reaction to obtain the eutectic electrolyte.

6. The method for preparing the eutectic electrolyte according to claim 5, characterized in that, The method for preparing the eutectic electrolyte precursor solution includes: mixing a hydrogen acceptor and a hydrogen donor under heating and stirring to obtain a first mixed solution; cooling the first mixed solution and adding an amide siloxane polymer monomer and mixing to obtain a second mixed solution; mixing the second mixed solution, a crosslinking agent, and an initiator to obtain the eutectic electrolyte precursor solution. And / or, the polymerization reaction includes ultraviolet light irradiation for 2 to 5 minutes.

7. An integrated solid-state negative electrode, characterized in that, include: A current collector and a negative electrode layer disposed on the surface of the current collector; the negative electrode layer includes a negative electrode active material, a conductive agent, a binder, a eutectic electrolyte as described in any one of claims 1 to 4, and an oxide solid electrolyte.

8. The integrated solid-state negative electrode according to claim 7, characterized in that, The mass of the eutectic electrolyte is 5% to 15% of the total mass of the negative electrode active material, the conductive agent, the binder, and the oxide solid electrolyte.

9. A solid-state battery, characterized in that, It includes the integrated solid-state negative electrode, positive electrode, and solid electrolyte as described in claim 7 or 8.

10. The solid-state battery according to claim 9, characterized in that, The solid electrolyte is mainly obtained by thermal polymerization of acrylate monomers, lithium salts, plasticizers, crosslinking agents and thermal initiators.

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