Hitherto, it remains a great challenge to stabilize the electrolyte–electrode interfaces and impede lithium dendrite proliferation in lithium metal batteries with high‐capacity nickel‐rich LiNxCoyMn1‐x‐yO2 (NCM) layer cathodes. Herein, a special molecular‐level designed polymer electrolyte is prepared by the copolymerization of hexafluorobutyl acrylate and methylene bisacrylamide to construct dual‐reinforced stable interfaces. Verified by X‐ray photoelectron spectroscopy depth profiling, there are favorable solid electrolyte interphase (SEI) layers on Li metal anodes and robust cathode electrolyte interphase (CEI) on Ni‐rich cathodes. The SEI enriched in lithiophilic N‐(C)3 guides the homogenous distribution of Li+ and facilitates the transport of Li+ through LiF and Li3N, promoting uniform Li+ plating and stripping. Moreover, the CEI with antioxidative amide groups could suppress the parasitic reactions between cathode and electrolyte and the structural degradation of cathode. Meanwhile, a unique two‐stage rheology‐tuning UV polymerization strategy is utilized, which is quite suited for continuous electrolyte fabrication with environmental friendliness. The fabricated polymer electrolyte exhibits a high ionic conductivity of 1.01 mS cm−1 at room temperature. 4.5 V NCM622//Li batteries achieve prolonged operation with a retention rate of 85.0% after 500 cycles at 0.5 C. This work provides new insights into molecular design and processibility design for polymer‐based high‐voltage batteries.This article is protected by copyright. All rights reserved
Lithium metal batteries with polyethylene oxide (PEO) electrolytes are considered as one of the ideal candidates for next generation power sources. However, the low ambient operation capability and conventional solvent‐based fabrication process of PEO limit their large‐scale application. In this work, a comb‐like quasi‐solid polymer electrolyte (QPE) reinforced with polyethylene glycol terephthalate nonwoven is fabricated. Combining the density functional theory calculation analysis and polymer structure design, optimized and synergized ion conductive channels are established by copolymerization of tetrahydrofurfuryl acrylate and introduction of plasticizer tetramethyl urea. Additionally, a unique two‐stage solventless UV polymerization strategy is utilized for rheology tuning and electrolyte fabrication. Compared with the conventional one‐step UV process, this strategy is ideally suited for the roll‐to‐roll continuous coating fabrication process with environmental friendliness. The fabricated QPE exhibits high ionic conductivity of 0.40 mS cm−1 and Li+ transference number (t = 0.77) at room temperature. LiFePO4//Li batteries are assembled to evaluate battery performance, which deliver excellent discharge capacity (144.9 mAh g−1 at 0.5 C) and cycling stability (with the retention rate 94.5% at 0.5 C after 200 cycles) at room temperature. The results demonstrate that it has high potential for solid‐state lithium metal batteries.
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