Preparation method of high-performance in-situ composite solid electrolyte containing dynamic covalent bonds

Abstract

The invention discloses a preparation method of a high-performance in-situ composite solid electrolyte containing a dynamic covalent bond. The high-performance in-situ composite solid electrolyte is prepared from the following raw materials: polymeric monomers of acrylics or a mixture thereof and the like, a polymer containing the dynamic covalent bond, an initiator, a lithium salt, a nano filler and an organic solvent. The dynamic covalent bond is introduced into the composite solid electrolyte, the migration ability of lithium ions in a polymer chain segment can be improved through breakage and recombination of the dynamic covalent bond, the lithium ion conductivity of the composite solid electrolyte is improved, and meanwhile, the polymer material containing the dynamic covalent bond can repair the solid-solid contact problem of the electrolyte and an electrode material in the cycle process; the stability and the cycle performance of the interface are greatly improved. The high-performance composite solid electrolyte is obtained by adding dynamic covalent bonds, and the rate, cycle and safety performance of the battery are improved.

Description

Technical Field

[0001] This invention relates to the field of battery technology, specifically to a method for preparing a high-performance in-situ composite solid electrolyte containing dynamic covalent bonds. Background Technology

[0002] Lithium-ion batteries are widely used in digital products and new energy vehicles due to their high energy density and low self-discharge characteristics. However, the energy density of traditional organic liquid electrolytes has reached its limit, and they are prone to fire and explosion accidents under extreme conditions, restricting the commercial application of high-capacity, high-energy lithium rechargeable batteries. Therefore, improving the safety and electrochemical performance of lithium-ion batteries, especially the design and development of high-performance electrolytes, is crucial.

[0003] Compared to traditional organic electrolytes, solid-state electrolytes offer significant safety advantages because they reduce the amount of flammable liquid components in lithium-ion batteries. However, solid-state electrolytes also face challenges such as high solid-solid interface impedance and low ionic conductivity, which affect the battery's charge-discharge performance and rate capability. Polymer solid-state electrolytes, due to their good flexibility and excellent interfacial contact characteristics, can significantly improve the safety and cycle performance of lithium-ion batteries. However, at room temperature, the low ionic conductivity of polymer solid-state electrolytes limits their industrial application.

[0004] To address these issues, researchers typically employ organic / inorganic composite solid-state electrolytes to improve interfacial contact and ionic conductivity in solid-state batteries. However, commonly used in-situ polymerized composite solid-state electrolytes exhibit low lithium-ion conductivity and poor electrode interface stability, leading to significant performance degradation in later stages of cycling. Therefore, there is a need to develop novel composite solid-state electrolytes to enhance ionic conductivity and interfacial stability, thereby improving the rate capability and cycle performance of semi-solid-state batteries. Summary of the Invention

[0005] The purpose of this invention is to provide a method for preparing a high-performance in-situ composite solid electrolyte containing dynamic covalent bonds, so as to solve the problems mentioned in the background art.

[0006] To achieve the above objectives, the present invention provides the following technical solution: a high-performance in-situ composite solid electrolyte containing dynamic covalent bonds, wherein the raw materials for preparing the in-situ solidified composite solid electrolyte include polymeric monomers of acrylates or mixtures thereof, polymers containing dynamic covalent bonds, initiators, lithium salts, nanofillers, and organic solvents.

[0007] Preferably, the polymeric monomers include any one or a combination of at least two of methacrylic acid, methyl methacrylate, 1,4-butanediol diacrylate, pentaerythritol tetraacrylate, and 2-carboxyethyl acrylate.

[0008] Preferably, the dynamic covalent bond is any one or a combination of at least two of the following: Diels-Alder reaction, disulfide bond, imine / acylhydrazone bond, and borate ester bond.

[0009] Preferably, the initiator includes any one or a combination of at least two of azobisisobutyronitrile, azobisisoheptanenitrile, and benzoyl peroxide.

[0010] Preferably, the lithium salt includes any one or a combination of two of lithium hexafluorophosphate and lithium bis(trifluoromethanesulfonyl)imide.

[0011] Preferably, the nanofiller includes any one or a combination of at least two of Al2O3, TiO2, and SiO2, and has a particle size of 10nm-500nm. Its nanostructure includes nanoparticles, nanowires, and nanosheets.

[0012] Preferably, the organic solvent includes any one or a combination of at least two of ethylene carbonate, dimethyl carbonate, and acetonitrile.

[0013] Preferably, the raw materials for preparing the in-situ solidified electrolyte further include additives; the additives include any one or a combination of at least two of vinylene carbonate, fluorovinyl carbonate, propylene sulfite, and ethylene sulfate.

[0014] Preferably, based on the total mass of the in-situ cured electrolyte precursor as 100%, the mass percentage of the polymeric monomer is 1%-40%, the mass percentage of the initiator is 0.01%-2%, the concentration of lithium salt in the in-situ cured electrolyte precursor is 1-3 mol / L, the mass percentage of the dynamically covalently bonded polymer is 0%-40% of the mass percentage of the polymeric monomer, the mass percentage of the nanofiller is 0.0005%-10% of the mass percentage of the polymeric monomer, and the mass percentage of the organic solvent is 60%-90%.

[0015] Preferably, a method for preparing a high-performance in-situ composite solid electrolyte containing dynamic covalent bonds is characterized by comprising the following steps: mixing a polymeric monomer, a polymer containing dynamic covalent bonds, an initiator, a lithium salt, a nanofiller, and an organic solvent to obtain an in-situ cured electrolyte precursor; injecting the precursor into a battery cell; encapsulating; allowing to stand; and heating to cure to obtain the in-situ cured composite solid electrolyte.

[0016] Compared with the prior art, the beneficial effects of the present invention are:

[0017] (1) The preparation method of this invention is simple and the reaction conditions are easy to control and achieve. When the dynamic covalent bond (boronic acid ester bond) is introduced in the first way, the crosslinking agent boric acid can be added during the preparation of the positive and negative electrode sheets. This not only makes the distribution of the dynamic covalent bond more uniform, but also benefits the processing performance of the ultra-high nickel cathode material.

[0018] (2) In this invention, the introduction of dynamic covalent bonds (boron ester bonds) enables the lithium ions of the lithium salt to rapidly dissociate and achieve dynamic migration of Li ions through Lewis acid-base interaction between boron atoms and salt anions, thereby improving the ionic conductivity of the composite solid electrolyte.

[0019] (3) In this invention, the introduction of dynamic covalent bonds (boronic acid ester bonds) gives the composite solid electrolyte a better three-dimensional network structure. At the same time, the dynamic ester exchange reaction of borate esters endows the composite solid electrolyte with super mechanical stability and self-healing properties, which greatly improves the solid-solid contact interface between the electrode material and the solid electrolyte and enhances the cycle performance of the semi-solid battery. Detailed Implementation

[0020] The technical solutions in the embodiments of the present invention will be clearly and completely described below. Obviously, the described embodiments are only some embodiments of the present invention, and not all embodiments. 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.

[0021] The present invention provides the following technical solution: a high-performance in-situ composite solid electrolyte containing dynamic covalent bonds, wherein the raw materials for preparing the in-situ solidified composite solid electrolyte include polymeric monomers of acrylates or mixtures thereof, polymers containing dynamic covalent bonds, initiators, lithium salts, nanofillers and organic solvents.

[0022] The preparation method includes the following steps: mixing a polymer monomer, a polymer containing dynamic covalent bonds, an initiator, a lithium salt, a nanofiller, and an organic solvent to obtain an in-situ solidified electrolyte precursor; injecting the precursor into a battery cell, encapsulating it, allowing it to stand, and heating it to solidify it to obtain the in-situ solidified composite solid electrolyte.

[0023] Example 1:

[0024] A method for preparing a semi-solid cylindrical battery with a high-performance in-situ composite solid electrolyte containing dynamic covalent bonds, characterized by comprising the following steps:

[0025] A. According to the formula of the positive and negative composite electrode sheet, first apply the binder, then add the conductive agent, solid electrolyte, positive electrode material, and negative electrode material in sequence into the mixing tank and stir evenly to obtain the positive and negative composite slurry respectively; (0.1% boric acid is added to the positive and negative electrode sheet formulas respectively)

[0026] B. The positive and negative electrode slurries are coated and dried to form positive and negative composite electrode sheets. The positive and negative electrode sheets are rolled, slit, cut, tab welded and wound to form cylindrical cells.

[0027] C. Then, the in-situ cured electrolyte precursor is injected into the cylindrical cell, and it is left to stand for 1 minute under a vacuum of -80 kPa. After laser welding the cap, it is left to stand for 48 hours in an environment of 20°C. Finally, it is cured for 12 hours in a rotatable in-situ curing device at 60°C to obtain an in-situ cured composite solid-state battery.

[0028] In this embodiment, the positive electrode material includes a nickel-cobalt-manganese ternary electrode; the negative electrode material includes a silicon-carbon negative electrode.

[0029] In this embodiment, the conductive agent includes a combination of Super LiP and carbon nanotubes.

[0030] In this embodiment, the binder includes a combination of polyvinylidene fluoride (PVDF) and polytetrafluoroethylene (PTFE).

[0031] In this embodiment, the solid electrolyte includes lithium lanthanum zirconium oxide (modified) with a particle size of 100-300 nm.

[0032] In this embodiment, the in-situ cured electrolyte precursor includes a polymeric monomer, an initiator, a lithium salt, a nanofiller, a dynamically covalent polymer (generated by the reaction of polyvinyl alcohol (PVA) and boric acid), and an organic solvent. The polymeric monomer accounts for 3% of the total mass, the initiator accounts for 0.2% of the total mass, the nanofiller accounts for 3% of the total mass of the polymeric monomer, the dynamically covalent polymer accounts for 5% of the total mass of the polymeric monomer, the lithium salt has a concentration of 1.2 mol / L, and the additive accounts for 8% of the total mass.

[0033] In this embodiment, the polymerizing monomers include pentaerythritol tetraacrylate and 2-carboxyethyl acrylate; the initiator includes a combination of azobisisobutyronitrile and azobisisoheptanenitrile; the lithium salt includes lithium hexafluorophosphate and lithium bis(trifluoromethanesulfonyl)imide; the nanofiller is nano-SiO2; and the dynamic covalent polymer is a borate ester polymer generated by the esterification reaction of PVA and boric acid.

[0034] In this embodiment, the in-situ cured electrolyte precursor also includes additives, which include a combination of vinylene carbonate and fluoroethylene carbonate.

[0035] Example 2:

[0036] A method for preparing a semi-solid cylindrical battery with a high-performance in-situ composite solid electrolyte containing dynamic covalent bonds, characterized by comprising the following steps:

[0037] A. According to the formula of the positive and negative composite electrode, first apply the binder, then add the conductive agent, solid electrolyte, positive electrode material, and negative electrode material in sequence into the mixing tank and stir evenly to obtain the positive and negative composite slurry respectively; (0.2% boric acid is added to the positive and negative electrode formulas respectively)

[0038] B. The positive and negative electrode slurries are coated and dried to form positive and negative composite electrode sheets. The positive and negative electrode sheets are rolled, slit, cut, tab welded and wound to form cylindrical cells.

[0039] C. Then, the in-situ cured electrolyte precursor is injected into the cylindrical cell, and it is left to stand for 1 minute under a vacuum of -80 kPa. After laser welding the cap, it is left to stand for 48 hours in an environment of 20°C. Finally, it is cured for 12 hours in a rotatable in-situ curing device at 60°C to obtain an in-situ cured composite solid-state battery.

[0040] In this embodiment, the positive electrode material includes a nickel-cobalt-manganese ternary electrode; the negative electrode material includes a silicon-carbon negative electrode.

[0041] In this embodiment, the conductive agent includes a combination of Super LiP and carbon nanotubes.

[0042] In this embodiment, the binder includes a combination of polyvinylidene fluoride (PVDF) and polytetrafluoroethylene (PTFE).

[0043] In this embodiment, the solid electrolyte includes lithium lanthanum zirconium oxide (modified) with a particle size of 100-300 nm.

[0044] In this embodiment, the in-situ cured electrolyte precursor includes a polymeric monomer, an initiator, a lithium salt, a nanofiller, a dynamically covalent polymer (generated by the reaction of polyvinyl alcohol (PVA) and boric acid), and an organic solvent. The polymeric monomer accounts for 3% of the total mass, the initiator accounts for 0.2% of the total mass, the nanofiller accounts for 3% of the total mass of the polymeric monomer, the dynamically covalent polymer accounts for 10% of the total mass of the polymeric monomer, the lithium salt has a concentration of 1.2 mol / L, and the additive accounts for 8% of the total mass.

[0045] In this embodiment, the polymerizing monomers include pentaerythritol tetraacrylate and 2-carboxyethyl acrylate; the initiator includes a combination of azobisisobutyronitrile and azobisisoheptanenitrile; the lithium salt includes lithium hexafluorophosphate and lithium bis(trifluoromethanesulfonyl)imide; the nanofiller is nano-SiO2; and the dynamic covalent polymer is a borate polymer generated by the reaction of PVA with borate esterification.

[0046] In this embodiment, the in-situ cured electrolyte precursor also includes additives, which include a combination of vinylene carbonate and fluoroethylene carbonate.

[0047] Example 3:

[0048] A method for preparing a semi-solid cylindrical battery with a high-performance in-situ composite solid electrolyte containing dynamic covalent bonds, characterized by comprising the following steps:

[0049] A. According to the formula of the positive and negative composite electrode, the binder is first applied, and then the conductive agent, solid electrolyte, positive electrode material and negative electrode material are added in sequence and stirred evenly in the mixing tank to obtain positive and negative composite slurry respectively.

[0050] B. The positive and negative electrode slurries are coated and dried to form positive and negative composite electrode sheets. The positive and negative electrode sheets are rolled, slit, cut, tab welded and wound to form cylindrical cells.

[0051] C. Then, the in-situ cured electrolyte precursor is injected into the cylindrical cell, and it is left to stand for 1 minute under a vacuum of -80 kPa. After laser welding the cap, it is left to stand for 48 hours in an environment of 20°C. Finally, it is cured for 12 hours in a rotatable in-situ curing device at 60°C to obtain an in-situ cured composite solid-state battery.

[0052] In this embodiment, the positive electrode material includes a nickel-cobalt-manganese ternary electrode; the negative electrode material includes a silicon-carbon negative electrode.

[0053] In this embodiment, the conductive agent includes a combination of Super LiP and carbon nanotubes.

[0054] In this embodiment, the binder includes a combination of polyvinylidene fluoride (PVDF) and polytetrafluoroethylene (PTFE).

[0055] In this embodiment, the solid electrolyte includes lithium lanthanum zirconium oxide (modified) with a particle size of 100-300 nm.

[0056] In this embodiment, the in-situ cured electrolyte precursor includes a polymeric monomer, an initiator, a lithium salt, a nanofiller, a dynamically covalent polymer, and an organic solvent. The polymeric monomer accounts for 3% of the total mass, the initiator accounts for 0.2% of the total mass, the nanofiller accounts for 3% of the total mass of the polymeric monomer, the dynamically covalent polymer accounts for 5% of the total mass of the polymeric monomer, the lithium salt has a concentration of 1.2 mol / L, and the additive accounts for 8% of the total mass.

[0057] In this embodiment, the polymerizing monomer includes pentaerythritol tetraacrylate; the initiator includes a combination of azobisisobutyronitrile and azobisisoheptanenitrile; the lithium salt includes lithium hexafluorophosphate and lithium bis(trifluoromethanesulfonyl)imide; the nanofiller is nano-SiO2; and the dynamic covalent polymer is any one or a combination of two of (2-hydroxy-5-methylphenyl)boronic acid ester and 1,3-propanediol 2-hydroxyphenylboronic acid ester.

[0058] In this embodiment, the in-situ cured electrolyte precursor also includes additives, which include a combination of vinylene carbonate and fluoroethylene carbonate.

[0059] Example 4:

[0060] A method for preparing a semi-solid cylindrical battery with a high-performance in-situ composite solid electrolyte containing dynamic covalent bonds, characterized by comprising the following steps:

[0061] A. According to the formula of the positive and negative composite electrode, the binder is first applied, and then the conductive agent, solid electrolyte, positive electrode material and negative electrode material are added in sequence and stirred evenly in the mixing tank to obtain positive and negative composite slurry respectively.

[0062] B. The positive and negative electrode slurries are coated and dried to form positive and negative composite electrode sheets. The positive and negative electrode sheets are rolled, slit, cut, tab welded and wound to form cylindrical cells.

[0063] C. Then, the in-situ cured electrolyte precursor is injected into the cylindrical cell, and it is left to stand for 1 minute under a vacuum of -80 kPa. After laser welding the cap, it is left to stand for 48 hours in an environment of 20°C. Finally, it is cured for 12 hours in a rotatable in-situ curing device at 60°C to obtain an in-situ cured composite solid-state battery.

[0064] In this embodiment, the positive electrode material includes a nickel-cobalt-manganese ternary electrode; the negative electrode material includes a silicon-carbon negative electrode.

[0065] In this embodiment, the conductive agent includes a combination of Super LiP and carbon nanotubes.

[0066] In this embodiment, the binder includes a combination of polyvinylidene fluoride (PVDF) and polytetrafluoroethylene (PTFE).

[0067] In this embodiment, the solid electrolyte includes lithium lanthanum zirconium oxide (modified) with a particle size of 100-300 nm.

[0068] In this embodiment, the in-situ cured electrolyte precursor includes a polymeric monomer, an initiator, a lithium salt, a nanofiller, a dynamically covalent polymer, and an organic solvent. The polymeric monomer accounts for 3% of the total mass, the initiator accounts for 0.2% of the total mass, the nanofiller accounts for 3% of the total mass of the polymeric monomer, the dynamically covalent polymer accounts for 10% of the total mass of the polymeric monomer, the lithium salt has a concentration of 1.2 mol / L, and the additive accounts for 8% of the total mass.

[0069] In this embodiment, the polymerizing monomer includes pentaerythritol tetraacrylate; the initiator includes a combination of azobisisobutyronitrile and azobisisoheptanenitrile; the lithium salt includes lithium hexafluorophosphate and lithium bis(trifluoromethanesulfonyl)imide; the nanofiller is nano-SiO2; and the dynamic covalent polymer is any one or a combination of two of (2-hydroxy-5-methylphenyl)boronic acid ester and 1,3-propanediol 2-hydroxyphenylboronic acid ester.

[0070] In this embodiment, the in-situ cured electrolyte precursor also includes additives, which include a combination of vinylene carbonate and fluoroethylene carbonate.

[0071] Experimental example:

[0072] A method for preparing a semi-solid cylindrical battery with a high-performance in-situ composite solid electrolyte containing dynamic covalent bonds, characterized by comprising the following steps:

[0073] A. According to the formula of the positive and negative composite electrode, the binder is first applied, and then the conductive agent, solid electrolyte, positive electrode material and negative electrode material are added in sequence and stirred evenly in the mixing tank to obtain positive and negative composite slurry respectively.

[0074] B. The positive and negative electrode slurries are coated and dried to form positive and negative composite electrode sheets. The positive and negative electrode sheets are rolled, slit, cut, tab welded and wound to form cylindrical cells.

[0075] C. Then, the in-situ cured electrolyte precursor is injected into the cylindrical cell, and it is left to stand for 1 minute under a vacuum of -80 kPa. After laser welding the cap, it is left to stand for 48 hours in an environment of 20°C. Finally, it is cured for 12 hours in a rotatable in-situ curing device at 60°C to obtain an in-situ cured composite solid-state battery.

[0076] In this embodiment, the positive electrode material includes a nickel-cobalt-manganese ternary electrode; the negative electrode material includes a silicon-carbon negative electrode.

[0077] In this embodiment, the conductive agent includes a combination of Super LiP and carbon nanotubes.

[0078] In this embodiment, the binder includes a combination of polyvinylidene fluoride (PVDF) and polytetrafluoroethylene (PTFE).

[0079] In this embodiment, the solid electrolyte includes lithium lanthanum zirconium oxide (modified) with a particle size of 100-300 nm.

[0080] In this embodiment, the in-situ cured electrolyte precursor includes a polymeric monomer, an initiator, a lithium salt, a nanofiller, and an organic solvent. The polymeric monomer has a mass percentage of 3%, the initiator has a mass percentage of 0.2%, the lithium salt has a concentration of 1.2 mol / L, and the additive has a mass percentage of 8%.

[0081] In this embodiment, the monomer includes pentaerythritol tetraacrylate; the initiator includes a combination of azobisisobutyronitrile and azobisisoheptanenitrile; the lithium salt includes lithium hexafluorophosphate and lithium bis(trifluoromethanesulfonyl)imide; and the nanofiller is nano-SiO2.

[0082] In this embodiment, the in-situ cured electrolyte precursor also includes additives, which include a combination of vinylene carbonate and fluoroethylene carbonate.

[0083] Conductivity test: The ionic conductivity of the semi-solid batteries made from the positive electrode sheets obtained from each application example was tested.

[0084] AC impedance: The AC impedance voltage signal of the batteries in each embodiment and comparative example was tested on an electrochemical workstation at a frequency range of 10 mV. 6 -10 -2 Hz, ionic conductivity is calculated from EIS results combined with the ionic conductivity formula; δ=L / RA (L is thickness, A is area, R is resistance).

[0085] The batteries prepared using the various embodiments of the present invention were subjected to performance testing, and the data obtained are shown in the table below:

[0086]

[0087]

[0088] In summary, the preparation method of this invention is simple, and the reaction conditions are easy to control and implement. When the dynamic covalent bond (boronate bond) is introduced in method one, the crosslinking agent boric acid can be added during the preparation of the positive and negative electrode sheets. This not only makes the distribution of the dynamic covalent bond more uniform but also benefits the processing performance of the ultra-high nickel cathode material. In this invention, the introduction of the dynamic covalent bond (boronate bond) enables the rapid dissociation of lithium ions in the lithium salt and the dynamic migration of Li ions through the Lewis acid-base interaction between boron atoms and salt anions, thereby improving the ionic conductivity of the composite solid electrolyte. In this invention, the introduction of the dynamic covalent bond (boronate bond) gives the composite solid electrolyte a better three-dimensional network structure. At the same time, the dynamic transesterification reaction of the boronate ester endows the composite solid electrolyte with superior mechanical stability and self-healing properties, greatly improving the solid-solid contact interface between the electrode material and the solid electrolyte and enhancing the cycle performance of the semi-solid battery.

[0089] Although embodiments of the invention have been shown and described, it will be understood by those skilled in the art that various changes, modifications, substitutions and alterations can be made to these embodiments without departing from the principles and spirit of the invention, the scope of which is defined by the appended claims and their equivalents.

Claims

1. A high-performance in-situ composite solid electrolyte containing dynamic covalent bonds, characterized in that: The raw materials for preparing the in-situ cured composite solid electrolyte include polymeric monomers of acrylates or mixtures thereof, polymers containing dynamic covalent bonds, initiators, lithium salts, nanofillers, and organic solvents.

2. The high-performance in-situ composite solid electrolyte containing dynamic covalent bonds according to claim 1, characterized in that: The polymer monomers include any one or a combination of at least two of the following: methacrylic acid, methyl methacrylate, 1,4-butanediol diacrylate, pentaerythritol tetraacrylate, and 2-carboxyethyl acrylate.

3. The high-performance in-situ composite solid electrolyte containing dynamic covalent bonds according to claim 1, characterized in that: The dynamic covalent bond is any one or a combination of at least two of the following: Diels-Alder reaction, disulfide bond, imine / acylhydrazone bond, and borate ester bond.

4. The high-performance in-situ composite solid electrolyte containing dynamic covalent bonds according to claim 1, characterized in that: The initiator includes any one or a combination of at least two of azobisisobutyronitrile, azobisisoheptanenitrile, and benzoyl peroxide.

5. The high-performance in-situ composite solid electrolyte containing dynamic covalent bonds according to claim 1, characterized in that: The lithium salt includes any one or a combination of two of lithium hexafluorophosphate and lithium bis(trifluoromethanesulfonyl)imide.

6. The high-performance in-situ composite solid electrolyte containing dynamic covalent bonds according to claim 1, characterized in that: The nanofiller includes any one or a combination of at least two of Al2O3, TiO2, and SiO2, and has a particle size of 10nm-500nm. Its nanostructure includes nanoparticles, nanowires, and nanosheets.

7. The high-performance in-situ composite solid electrolyte containing dynamic covalent bonds according to claim 1, characterized in that: The organic solvent includes any one or a combination of at least two of ethylene carbonate, dimethyl carbonate, and acetonitrile.

8. The high-performance in-situ composite solid electrolyte containing dynamic covalent bonds according to claim 1, characterized in that: The raw materials for preparing the in-situ solidified electrolyte also include additives; the additives include any one or a combination of at least two of vinylene carbonate, fluorovinyl carbonate, propylene sulfite, and ethylene sulfate.

9. A high-performance in-situ composite solid electrolyte containing dynamic covalent bonds according to claim 1, characterized in that: Based on the total mass of the in-situ cured electrolyte precursor as 100%, the mass percentage of the polymeric monomer is 1%-40%, the mass percentage of the initiator is 0.01%-2%, the concentration of lithium salt in the in-situ cured electrolyte precursor is 1-3 mol / L, the mass percentage of the dynamically covalently bonded polymer is 0%-40% of the mass percentage of the polymeric monomer, the mass percentage of the nanofiller is 0.0005%-10% of the mass percentage of the polymeric monomer, and the mass percentage of the organic solvent is 60%-90%.

10. A method for preparing a high-performance in-situ composite solid electrolyte containing dynamic covalent bonds as described in any one of claims 1-9, characterized in that, Includes the following steps: A polymeric monomer, a polymer containing dynamic covalent bonds, an initiator, a lithium salt, a nanofiller, and an organic solvent are mixed to obtain an in-situ cured electrolyte precursor. The precursor is injected into a battery cell, encapsulated, left to stand, and then cured by heating to obtain the in-situ cured composite solid electrolyte.

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