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Herein, a special molecular\u2010level\u2010designed polymer electrolyte is prepared by the copolymerization of hexafluorobutyl acrylate and methylene bisacrylamide to construct dual\u2010reinforced stable interfaces. Verified by X\u2010ray photoelectron spectroscopy depth profiling, there are favorable solid electrolyte interphase (SEI) layers on Li metal anodes and robust cathode electrolyte interphase (CEI) on Ni\u2010rich cathodes. The SEI enriched in lithiophilic N\u2212(C)<jats:sub>3<\/jats:sub> guides the homogenous distribution of Li<jats:sup>+<\/jats:sup> and facilitates the transport of Li<jats:sup>+<\/jats:sup> through LiF and Li<jats:sub>3<\/jats:sub>N, promoting uniform Li<jats:sup>+<\/jats:sup> plating and stripping. Moreover, the CEI with antioxidative amide groups can suppress the parasitic reactions between cathode and electrolyte and the structural degradation of cathode. Meanwhile, a unique two\u2010stage rheology\u2010tuning 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<jats:sup>\u22121<\/jats:sup> at room temperature. 4.5\u00a0V 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\u2010based high\u2010voltage batteries.<\/jats:p>","DOI":"10.1002\/adma.202304951","type":"journal-article","created":{"date-parts":[[2023,7,19]],"date-time":"2023-07-19T13:20:17Z","timestamp":1689772817000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":128,"title":["Enabling Scalable Polymer Electrolyte with Dual\u2010Reinforced Stable Interface for 4.5\u00a0V Lithium\u2010Metal Batteries"],"prefix":"10.1002","volume":"35","author":[{"given":"Shengguang","family":"Qi","sequence":"first","affiliation":[{"name":"Guangdong Provincial Key Laboratory of Fuel Cell Technology School of Chemistry and Chemical Engineering South China University of Technology  Guangzhou 510641 China"},{"name":"School of Materials Science and Engineering South China University of Technology  Guangzhou 510641 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