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To address these safety concerns, an electron beam (E\u2010beam)\u2010induced gel polymer electrolyte (E\u2010Gel) is introduced, employing dipentaerythritol hexaacrylate (DPH) as a bi\u2010functional cross\u2013linkable additive (CIA). The dual roles of DPH are exploited through a strategically designed E\u2010beam irradiation process. Applying E\u2010beam irradiation on the pre\u2010cycled cells allows DPH to function as an additive during the initial cycle, establishing a protective layer on the surface of the anode and cathode and as a cross\u2013linker during the E\u2010beam irradiation step, forming a polymer framework. The prepared E\u2010Gel with CIA has superior interfacial compatibility, facilitating lithium\u2010ion diffusion at the electrode\/E\u2010Gel interface. The electrochemical assessment of 1.2 Ah pouch cells demonstrates that E\u2010Gel substantially reduces gas release by 2.5 times compared to commercial LEs during the initial formation stage and ensures superior reversible capacity retention even after prolonged cycling at 55\u00a0\u00b0C. The research underscores the synergy of bifunctional CIA with E\u2010beam technology, paving the way for large\u2010scale production of safe, high\u2010capacity, and commercially viable LIBs.<\/jats:p>","DOI":"10.1002\/smll.202401426","type":"journal-article","created":{"date-parts":[[2024,4,30]],"date-time":"2024-04-30T06:05:30Z","timestamp":1714457130000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Mitigating Gas Evolution in Electron Beam\u2010Induced Gel Polymer Electrolytes Through Bi\u2010Functional Cross\u2013Linkable Additives"],"prefix":"10.1002","volume":"20","author":[{"given":"Seoha","family":"Nam","sequence":"first","affiliation":[{"name":"Department of Chemistry Pohang University of Science and Technology (POSTECH)  Pohang 37673 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hye Bin","family":"Son","sequence":"additional","affiliation":[{"name":"Department of 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