A polymer battery and a preparation method and application thereof

Abstract

This invention discloses a polymer battery, its preparation method, and its application. The preparation method of the polymer battery includes the following steps: S1. Coating an electrode slurry containing a first polymerizable monomer onto a current collector, and drying it to form a coating, thus obtaining an electrode sheet; S2. Assembling a battery using an electrolyte and the electrode sheet obtained in step S1, and after injecting the electrolyte, allowing it to stand at 35~65°C to wet the coating of the electrode sheet obtained in step S1 with the electrolyte, and then undergoing a polymerization reaction at 70~120°C to obtain the polymer battery. The polymer battery obtained by this invention has a chemically anchored three-dimensional cross-linked network at the electrode-electrolyte interface, resulting in stronger bonding at the electrode-electrolyte interface, making it less prone to interface failure during long-term cycling, exhibiting excellent electrical performance, and also possessing good long-term heat resistance.

Description

Technical Field

[0001] This invention belongs to the field of polymer electrolytes, specifically relating to a polymer battery, its preparation method, and its application. Background Technology

[0002] With the acceleration of global energy structure transformation and electrification, lithium-ion batteries have become the core power source for portable electronic devices, electric vehicles, and large-scale energy storage systems due to their advantages such as high energy density and long lifespan. Among these, gel batteries, by immobilizing a liquid electrolyte within a three-dimensional polymer network, form a gel electrolyte that combines the safety of solid-state electrolytes with the high ionic conductivity of liquid electrolytes. Compared to traditional liquid or solid polymer batteries, it offers both higher conductivity and safety, making it a crucial technology in the battery field. A typical gel battery consists of a positive electrode, a negative electrode, a separator, and a gel electrolyte. Its performance largely depends on the interfacial stability between these components, especially between the electrodes and the gel electrolyte.

[0003] However, gel batteries face a key challenge during long-term cycling: weak interfacial bonding between the electrodes and the gel electrolyte. During charge and discharge, the electrode active materials (such as silicon-based anodes and high-nickel cathodes) undergo repeated volume expansion and contraction, generating continuous mechanical stress. Under this stress, micro-gaps form at the interface between the electrodes and the gel electrolyte. This not only disrupts ion transport pathways and drastically increases interfacial impedance and intensifies battery polarization, but also exacerbates internal side reactions. All of these factors contribute to accelerated capacity decay and a significantly shortened lifespan during long-term cycling.

[0004] Existing technologies have made numerous attempts to optimize the electrode-electrolyte contact. For example, Chinese patent CN114843434 describes an electrode sheet, solid-state battery, and electronic device, which coats the surface of the battery electrode sheet with a functional coating containing a gel electrolyte. The gel electrolyte on the electrode surface provides additional ion conduction pathways and buffers volume changes, thereby optimizing the electrode-electrolyte interface contact and improving the battery's long-term cycle performance. However, this existing technology still does not solve the problem of weak interfacial bonding between the electrode and electrolyte, and the battery's cycle life and long-term cycle performance still need improvement. Summary of the Invention

[0005] To address the problem of weak electrode-electrolyte interface bonding in existing gel batteries, which leads to shortened cycle life and poor long-term cycle performance, this invention provides a method for preparing polymer batteries that improves electrode-electrolyte interface bonding, resulting in polymer batteries with longer cycle life and excellent long-term cycle performance.

[0006] Another object of the present invention is to provide a polymer battery.

[0007] The above-mentioned objective of the present invention is achieved through the following technical solution: A method for preparing a polymer battery includes the following steps: S1. The electrode slurry containing the first polymerizable monomer is coated onto the current collector, and dried to form a coating, thus obtaining the electrode sheet; S2. Assemble a battery using an electrolyte and the electrode sheet described in step S1, and after injecting the electrolyte, let it stand at 35~65°C to allow the coating of the electrode sheet described in step S1 to be wetted by the electrolyte, and then allow a polymerization reaction to occur at 70~120°C to obtain a polymer battery. Step S1: The first polymerizable monomer contains at least two carbon-carbon unsaturated bonds; The electrolyte in step S2 contains an initiator and a second polymerizable monomer; the initiation temperature of the initiator is 70~120°C; the second polymerizable monomer contains at least one carbon-carbon unsaturated bond; the positive and / or negative electrode of the polymer battery is the electrode sheet in step S1.

[0008] It should be noted that: This invention involves coating an electrode slurry (containing a specific first polymerizable monomer, without an initiator) onto the current collector of an electrode sheet to form a coating, thereby producing an electrode sheet with the aforementioned specific first polymerizable monomer incorporated into the coating. This electrode sheet is then used as the positive and / or negative electrode, assembled into a battery with an electrolyte containing an initiator. The battery is first allowed to stand at 35-65°C to allow the coating to be wetted by the electrolyte, followed by a polymerization reaction at 70-120°C. This process results in a polymer battery with a stronger bonding force at the electrode-electrolyte interface, making the interface less prone to failure during long-term cycling, maintaining excellent electrical performance, and exhibiting good long-term heat resistance. The principle is as follows: During the polymerization reaction described above, the first polymerizable monomer in the electrode coating of this invention can polymerize simultaneously with the initiator in the electrolyte (whose initiation temperature is compatible with the polymerization reaction temperature). Since each molecule of the first polymerizable monomer contains at least two carbon-carbon unsaturated bonds, a three-dimensional cross-linked network can be formed at the electrode-electrolyte interface. The presence of this three-dimensional cross-linked network significantly enhances the bonding force at the electrode-electrolyte interface, thereby enabling the polymer battery to maintain excellent electrical performance during long-term cycling and also exhibiting good long-term heat resistance. If the electrode coating does not contain the first polymerizable monomer, or if the number of carbon-carbon unsaturated bonds in the first polymerizable monomer is less than two, a three-dimensional cross-linked network cannot be formed, resulting in poor bonding force at the electrode-electrolyte interface. Consequently, the polymer battery produced will struggle to maintain its performance during long-term cycling, and its long-term heat resistance will also deteriorate. Similarly, if the initiator is added to the electrode coating instead of the electrolyte, a three-dimensional cross-linked network cannot be formed at the electrode-electrolyte interface, also leading to poor bonding force at the electrode-electrolyte interface.

[0009] Furthermore, prior to the polymerization reaction, the assembled battery is allowed to stand at 35-65°C to allow the electrode coating to be immersed in the electrolyte. This process helps increase the contact area between the electrolyte and the electrode, promoting the formation of the subsequent three-dimensional cross-linked network and thus enhancing the bonding force at the electrode-electrolyte interface. If the standing step is omitted, or if the standing time is too short to allow sufficient wetting and contact between the electrolyte and the electrode, the contact will be insufficient, hindering the formation of the three-dimensional cross-linked network and resulting in poor bonding force at the electrode-electrolyte interface.

[0010] Preferably, the electrode slurry in step S1 further comprises an electrode active material, a conductive agent, a binder, and an organic solvent.

[0011] More preferably, in the electrode slurry described in step S1, the mass ratio of the first polymerizable monomer, the electrode active material, the conductive agent, the binder, and the organic solvent is 1:(40~50):(0.8~1.2):(0.8~1.2):(30~35).

[0012] More preferably, the electrode active material is a high-nickel ternary material.

[0013] Commonly used high-nickel ternary materials in this field can all be used as the high-nickel ternary materials of this invention; specifically, including but not limited to LiNi. 0.8 Co 0.1 Mn 0.1 O2 (NCM811), LiNi 0.85 Co 0.1 Mn 0.05O2 (NCM851005), LiNi 0.9 Co 0.05 Mn 0.05 O2 (NCM900505), LiNi 0.95 Co 0.02 Mn 0.03 O2 (NCM950203), LiNi 0.8 Co 0.15 Al 0.05 O2 (NCA81505), LiNi 0.9 Co 0.05 Al 0.05 O2 (NCA90505).

[0014] More preferably, the conductive agent is at least one of carbon black, conductive graphite, carbon nanotubes (CNTs), graphene, and conductive fiber (VGCF).

[0015] More preferably, the adhesive is at least one of polyvinylidene fluoride (PVDF), polyvinylidene fluoride-hexafluoropropylene copolymer (PVDF-HFP), polyacrylic acid (PAA), and polyimide (PI).

[0016] More preferably, the organic solvent is at least one of N-methylpyrrolidone (NMP), N,N-dimethylformamide (DMF), N,N-dimethylacetamide (DMAc), and γ-butyrolactone (GBL).

[0017] More preferably, the mass ratio of electrode active material, crosslinking agent, conductive agent and binder in the electrode slurry in step S1 is 94:(0.5~2.5):(1.5~2.5):(1.5~2.5).

[0018] More preferably, the solid content of the electrode slurry in step S1 is 50~85wt%.

[0019] Preferably, in step S1, the first polymerizable monomer is at least one of (meth)acrylate compounds, vinyl compounds, or maleimide compounds.

[0020] More preferably, the polymerizable monomer is at least one selected from the following: tripropylene glycol diacrylate, 1,6-hexanediol diacrylate, pentaerythritol triacrylate, trimethylolpropane triacrylate (TMPTA), dipentaerythritol hexaacrylate (DPHA), bisphenol A hexafluoroacrylate (BPAF-DA), ethylene glycol dimethacrylate (EGDMA), and N,N'-m-phenylenebismaleimide (PDM).

[0021] Preferably, after coating in step S1, the process further includes drying, rolling, and cutting.

[0022] Preferably, in the coating described in step S1, the polymerizable monomer accounts for 0.02 to 8 wt% of the coating.

[0023] Preferably, the second polymerizable monomer is at least one selected from triethylene glycol diacrylate (TEGDA), polyethylene glycol dimethacrylate (PEGDMA), perfluorooctyl ethyl acrylate (PFOEA), N,N'-methylenebisacrylamide (MBA), and 1,4-butanediol dimethacrylate (BDDMA).

[0024] Preferably, the electrolyte in step S2 further comprises an electrolyte salt and an electrolyte solvent.

[0025] More preferably, in the electrolyte of step S2, the mass ratio of the second polymerizable monomer, initiator, electrolyte salt, and electrolyte solvent is 1:(0.2~0.3):(2.8~4.2):(20~30).

[0026] More preferably, the electrolyte salt is at least one selected from lithium hexafluorophosphate, lithium bis(fluorosulfonyl)imide, lithium bis(trifluoromethanesulfonyl)imide, lithium tetrafluoroborate, lithium difluorophosphate, and lithium hexafluoroantimonyate.

[0027] More preferably, the electrolyte solvent is at least one of ethylene carbonate and ethyl methyl carbonate.

[0028] More preferably, the electrolyte solvent is a mixture of ethylene carbonate and methyl ethyl carbonate in a volume ratio of 3:(6.5~7.5).

[0029] Preferably, the initiator is an organic peroxide initiator.

[0030] More preferably, the initiator is at least one of di-tert-butyl hydroperoxide and dicumyl peroxide.

[0031] Preferably, the settling time in step S2 is 8 to 18 hours.

[0032] More preferably, the settling time in step S2 is 12 to 18 hours.

[0033] Preferably, the polymerization reaction in step S2 takes 2 to 12 hours.

[0034] Preferably, both the settling and polymerization reactions in step S2 are carried out in an inert gas atmosphere.

[0035] More preferably, the inert gas is one of helium, neon, or argon.

[0036] The present invention also protects a polymer battery prepared by the above-described method.

[0037] Preferably, the battery is a lithium battery.

[0038] Compared with the prior art, the beneficial effects of the present invention are: This invention introduces a functional coating containing a specific crosslinking agent onto the surface of the electrode sheet of a polymer battery, and simultaneously introduces a specific initiator into the electrolyte. Then, using a synthesis step of first allowing the mixture to stand at a low temperature and then polymerizing it at a high temperature, the resulting polymer battery has a chemically anchored three-dimensional crosslinked network at the electrode-electrolyte interface. This polymer battery has stronger bonding at the electrode-electrolyte interface, is less prone to interface failure during long-term cycling, exhibits excellent electrical performance, and also has good long-term heat resistance. Detailed Implementation

[0039] The present invention will be further illustrated below with reference to specific embodiments, but the embodiments do not limit the present invention in any way. Unless otherwise specified, the reagents, methods, and equipment used in the present invention are conventional reagents, methods, and equipment in this technical field.

[0040] Unless otherwise specified, all reagents and materials used in the following examples are commercially available.

[0041] Example 1 This embodiment provides a method for preparing a polymer battery, comprising the following steps: (1) 15.0g of electrode active material LiNi 0.8 Co 0.1 Mn 0.1 O2 (NCM811, S85E, Ningbo Ronbay New Energy Technology Co., Ltd.), 0.32g conductive agent carbon black (Super P, TMEGO Ltd., Belgium), 0.32g binder polyvinylidene fluoride (PVDF 5130, Synesqo, number average molecular weight 1 million to 1.25 million) and 0.32g tripropylene glycol diacrylate (CAS: 42978-66-5) were mixed, and then 10.64g N-methylpyrrolidone (CAS: 872-50-4) solvent was added and stirred to prepare an electrode slurry. The slurry was uniformly coated onto a 12μm thick aluminum foil (AL-1060, Aluminum Corporation of China Limited) using a comma-shaped scraper, dried at 110℃ for 2 hours, rolled under 12MPa pressure, and cut to form electrode sheets (coating thickness 100μm). (2) Using the electrode sheet from step (1) as the positive electrode, copper foil as the negative electrode, and a porous polypropylene membrane (PP25um, Xingyuan material, thickness 25μm, porosity 42%) as the separator, a soft-pack battery is assembled in an argon glove box, and then the electrolyte is injected and sealed. Then the battery after electrolyte injection is placed in a constant temperature box at 45°C and kept at the temperature for 12h. The battery is then transferred to a constant temperature box at 85°C and kept at the temperature for 4h again to obtain a polymer battery. The electrolyte preparation process is as follows: 15.2g of lithium hexafluorophosphate (CAS: 21324-40-3), 4.5g of triethylene glycol diacrylate (CAS: 1680-21-3), 107.5g of mixed solvent (a mixture of ethylene carbonate and methyl ethyl carbonate in a volume ratio of 3:7), and 1.2g of dicumyl peroxide (CAS: 80-43-3) are mixed in an argon glove box with a moisture and oxygen content of less than 0.1 ppm, and magnetically stirred at 500 r / min for 2 h to obtain the electrolyte.

[0042] Example 2 This embodiment provides a method for preparing a polymer battery, which differs from Embodiment 1 in that: in step (1), tripropylene glycol diacrylate is replaced with an equal mass of 1,6-hexanediol diacrylate (CAS: 13048-33-4).

[0043] Example 3 This embodiment provides a method for preparing a polymer battery, which differs from Embodiment 1 in that: in step (1), dipropylene glycol diacrylate is replaced with an equal mass of pentaerythritol triacrylate (CAS: 3524-68-3).

[0044] Example 4 This embodiment provides a method for preparing a polymer battery, which differs from Embodiment 1 in that: in step (1), tripropylene glycol diacrylate is replaced with an equal mass of N,N'-m-phenylenebismaleimide (CAS: 3006-93-7).

[0045] Example 5 This embodiment provides a method for preparing a polymer battery, which differs from Embodiment 1 in that: in step (2), dicumyl peroxide is replaced with an equal mass of di-tert-butyl hydrogen peroxide (CAS: 110-05-4); the temperature for heat preservation and static setting is 105°C and the time is 4 hours.

[0046] Example 6 This embodiment provides a method for preparing a polymer battery, which differs from Embodiment 1 in that: in step (2), the temperature of the first heat preservation and static setting is 35°C and the time is 18h; in step (2), the temperature of the second heat preservation and static setting is 120°C and the time is 2h.

[0047] Example 7 This embodiment provides a method for preparing a polymer battery, which differs from Embodiment 1 in that: in step (2), the temperature of the first heat preservation and static setting is 65°C and the time is 8h; the temperature of the second heat preservation and static setting is 80°C and the time is 12h.

[0048] Example 8 This embodiment provides a method for preparing a polymer battery, which differs from Embodiment 1 in that the amount of tripropylene glycol diacrylate used is 0.08g.

[0049] Example 9 This embodiment provides a method for preparing a polymer battery, which differs from Embodiment 1 in that the amount of tripropylene glycol diacrylate used is 0.40g.

[0050] Example 10 This embodiment provides a method for preparing a polymer battery, which differs from Embodiment 1 in that: in step (2), the battery is assembled using the electrode sheet from step (1) as the negative electrode and the copper foil as the positive electrode.

[0051] Comparative Example 1 This comparative example provides a method for preparing a polymer battery, which differs from Example 1 in that: in step (1), dipropylene glycol diacrylate is not added.

[0052] Comparative Example 2 This comparative example provides a method for preparing a polymer battery, which differs from Example 1 in that: in step (1), tripropylene glycol diacrylate is replaced with an equal mass of methyl methacrylate (CAS: 80-62-6).

[0053] Comparative Example 3 This comparative example provides a method for preparing a polymer battery, which differs from Example 1 in that: in step (2), dicumyl peroxide is replaced with an equal mass of azobisisobutyronitrile (CAS: 78-67-1).

[0054] Comparative Example 4 This comparative example provides a method for preparing a polymer battery, which differs from Example 1 in that: in step (2), the step of keeping the battery warm and stationary after liquid injection is omitted.

[0055] Comparative Example 5 This comparative example provides a method for preparing a polymer battery, which differs from Example 1 in that: tripropylene glycol diacrylate is not added in step (1), but is mixed with the raw materials of the electrolyte in step (2) when preparing the electrolyte.

[0056] Comparative Example 6 This comparative example provides a method for preparing a polymer battery, which differs from Example 1 in that step (1) is adjusted to: 15.0g of electrode active material LiNi 0.8 Co 0.1 Mn 0.1 O2 (NCM811, S85E, Ningbo Ronbay New Energy Technology Co., Ltd.), 0.32g conductive agent carbon black (Super P, TMEGO Ltd., Belgium), 0.32g binder polyvinylidene fluoride (PVDF 5130, Synesqo, number average molecular weight 1 million to 1.25 million), 0.32g tripropylene glycol diacrylate and 1.2g dicumyl peroxide were mixed, and then 10.64g N-methylpyrrolidone solvent was added and stirred to prepare an electrode slurry. The slurry was uniformly coated onto a 12μm thick aluminum foil (AL-1060, Aluminum Corporation of China Limited) using a comma-shaped scraper. After drying at 110℃ for 2 hours, it was rolled under 12MPa pressure and cut to form an electrode sheet (coating thickness of 100μm). Then, the prepared electrode sheet was kept in a constant temperature oven at 85℃ for 4 hours to trigger polymerization.

[0057] Comparative Example 7 This comparative example provides a method for preparing a polymer battery, which differs from Example 10 in that: in step (1), dipropylene glycol diacrylate is not added.

[0058] Comparative Example 8 This comparative example provides a method for preparing a polymer battery, which differs from Example 1 in that: in step (2), the first heat preservation and standing time is 4 hours.

[0059] Performance testing The polymer batteries obtained in each embodiment and comparative example were subjected to performance testing, and the testing methods are as follows: (1) Interface peel strength: The peel force between the electrode sheet and the polymer electrolyte membrane separated from the cycled battery was measured using a universal testing machine with a 180° peel method, and the unit was N / m; (2) Capacity retention rate after 500 cycles: The battery was charged at 25°C with a constant current of 0.5C to 4.2V, charged with a constant voltage to ≤0.05C, and then discharged with a constant current of 0.5C to 3.0V. This constitutes one cycle. The discharge capacity of the first and 500th cycles was recorded, and the capacity retention rate was calculated. (3) Interfacial impedance growth after 500 cycles: Using an electrochemical workstation, the interfacial impedance before cycling (Rint-initial) and the interfacial impedance after 500 cycles (Rint-after) were measured in the frequency range of 100kHz to 0.01Hz. The difference in interfacial impedance before and after cycling was calculated, which is the interfacial impedance growth (ΔRint). (4) High-temperature storage test: After the battery is fully charged, it is stored in a 60°C constant temperature chamber for 7 days. After cooling to 25°C, the change in battery thickness is measured and the thickness expansion rate is calculated; and one charge-discharge cycle is performed to calculate the capacity recovery rate.

[0060] The performance test results (interface peel strength, capacity retention after 500 cycles, interface impedance growth after 500 cycles, and high-temperature storage capacity recovery rate) of each embodiment and comparative example are shown in Table 1.

[0061] Table 1 Performance test results of each embodiment and comparative example

[0062] As shown in Table 1, the interfacial peel strength of the polymer batteries in Examples 1-10 is not less than 7.2 N / m; the capacity retention after 500 cycles is not less than 84.0%; and the interfacial impedance increase is not greater than 24.5 Ω·cm. 2 The capacity recovery rate after high-temperature storage is no less than 89.5%, and the thickness expansion rate is no more than 6.8%. This indicates that the polymer battery prepared by this invention has strong electrode-electrolyte interface bonding, maintains excellent electrical performance under long-term cycling, and also has good long-term heat resistance.

[0063] In Comparative Example 1, the electrode coating did not contain the first polymerizable monomer, tripropylene glycol diacrylate. The resulting polymer battery had lower electrode-electrolyte interface peel strength, lower capacity retention after 500 cycles, greater interface impedance growth, lower capacity recovery after high-temperature storage, and greater thickness expansion. In Comparative Example 2, the first polymerizable monomer in the electrode coating was replaced with methyl methacrylate. The resulting polymer battery had lower electrode-electrolyte interface peel strength, lower capacity retention after 500 cycles, greater interface impedance growth, and greater thickness expansion after high-temperature storage. The initiator type in Comparative Example 3 was not selected appropriately, resulting in low electrode-electrolyte interface peel strength, low capacity retention after 500 cycles, large increase in interface impedance, low capacity recovery after high-temperature storage, and large thickness expansion rate in the polymer battery. Comparative Example 4 did not keep the battery warm and stationary after electrolyte injection. The polymer battery prepared had low electrode-electrolyte interface peel strength, low capacity retention after 500 cycles, large increase in interface impedance, and large thickness expansion rate. In Comparative Example 5, the first polymerizable monomer was not added to the electrode coating but to the electrolyte. The polymer battery prepared had lower electrode-electrolyte interface peel strength, lower capacity retention after 500 cycles, larger increase in interface impedance, lower capacity recovery after high-temperature storage, and larger thickness expansion rate. Comparative Example 6 did not add the initiator to the electrolyte, but added it to the electrode coating and pre-completed the polymerization of the electrode coating. The polymer battery prepared had low electrode-electrolyte interface peel strength, low capacity retention after 500 cycles, large interfacial impedance growth, and large thickness expansion rate. The negative electrode of Comparative Example 7 contains a coating, but the first polymerizable monomer, tripropylene glycol diacrylate, is not added to the negative electrode coating. The resulting polymer battery has low electrode-electrolyte interface peel strength, low capacity retention after 500 cycles, large increase in interface impedance, low capacity recovery after high-temperature storage, and large thickness expansion rate. Comparative Example 8 showed that the battery was kept warm and stationary for too short a time after electrolyte injection, and the coating of the electrode sheet was not wetted. As a result, the polymer battery had low electrode sheet-electrolyte interface peel strength, low capacity retention after 500 cycles, large increase in interface impedance, low capacity recovery rate after high temperature storage, and large thickness expansion rate.

[0064] Obviously, the above embodiments of the present invention are merely examples for clearly illustrating the present invention, and are not intended to limit the implementation of the present invention. Those skilled in the art can make other variations or modifications based on the above description. It is neither necessary nor possible to exhaustively describe all embodiments here. Any modifications, equivalent substitutions, and improvements made within the spirit and principles of the present invention should be included within the scope of protection of the claims of the present invention.

Claims

1. A method for preparing a polymer battery, characterized in that, Includes the following steps: S1. The electrode slurry containing the first polymerizable monomer is coated onto the current collector, and dried to form a coating, thus obtaining the electrode sheet; S2. Assemble a battery using an electrolyte and the electrode sheet described in step S1, and after injecting the electrolyte, let it stand at 35~65°C to allow the coating of the electrode sheet described in step S1 to be wetted by the electrolyte, and then allow a polymerization reaction to occur at 70~120°C to obtain a polymer battery. Step S1: The first polymerizable monomer contains at least two carbon-carbon unsaturated bonds; The electrolyte in step S2 contains an initiator and a second polymerizable monomer; the initiation temperature of the initiator is 70~120°C; the second polymerizable monomer contains at least one carbon-carbon unsaturated bond; the positive and / or negative electrode of the polymer battery is the electrode sheet in step S1.

2. The preparation method according to claim 1, characterized in that, The electrode slurry described in step S1 further comprises electrode active material, conductive agent, binder and organic solvent.

3. The preparation method according to claim 1, characterized in that, Step S1: The first polymerizable monomer is at least one of (meth)acrylate compounds, vinyl compounds, or maleimide compounds.

4. The preparation method according to claim 3, characterized in that, Step S1 The first polymerizable monomer is at least one of the following: tripropylene glycol diacrylate, 1,6-hexanediol diacrylate, pentaerythritol triacrylate, trimethylolpropane triacrylate, dipentaerythritol hexaacrylate, hexafluorobisphenol A diacrylate, ethylene glycol dimethacrylate, and N,N'-m-phenylenebismaleimide.

5. The preparation method according to claim 1, characterized in that, In the coating described in step S1, the first polymerizable monomer accounts for 0.02~8 wt% of the coating.

6. The preparation method according to claim 1, characterized in that, The settling time in step S2 is 8~18 hours.

7. The preparation method according to claim 1, characterized in that, The polymerization reaction in step S2 takes 2 to 12 hours.

8. The preparation method according to claim 1, characterized in that, The initiator is an organic peroxide initiator.

9. The preparation method according to claim 8, characterized in that, The initiator is at least one of di-tert-butyl hydroperoxide and dicumyl peroxide.

10. A polymer battery, characterized in that, It is prepared by any one of the preparation methods described in claims 1 to 9.

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