{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,9,28]],"date-time":"2026-09-28T13:02:03Z","timestamp":1790600523190,"version":"4.1.0"},"reference-count":53,"publisher":"Wiley","license":[{"start":{"date-parts":[[2026,9,28]],"date-time":"2026-09-28T00:00:00Z","timestamp":1790553600000},"content-version":"vor","delay-in-days":0,"URL":"http:\/\/creativecommons.org\/licenses\/by-nc\/4.0\/"},{"start":{"date-parts":[[2026,9,28]],"date-time":"2026-09-28T00:00:00Z","timestamp":1790553600000},"content-version":"tdm","delay-in-days":0,"URL":"http:\/\/doi.wiley.com\/10.1002\/tdm_license_1.1"}],"content-domain":{"domain":["onlinelibrary.wiley.com"],"crossmark-restriction":true},"short-container-title":["Angew Chem Int Ed"],"abstract":"<jats:title>ABSTRACT<\/jats:title>\n                  <jats:p>\n                    In\u2010situ gel polymer electrolytes (GPEs) have attracted attention as promising candidates for next\u2010generation lithium\u2010ion batteries, offering superior interfacial compatibility and enhanced safety compared with conventional liquid electrolytes. However, the issue of residual monomers remaining after polymerization has not been adequately addressed. They readily decompose at the high\u2010Ni cathode (NCM) surface during the early stage of formation, generating an organic\u2010rich layer within the inner cathode\u2013electrolyte interphase (CEI) and disrupting the normal CEI\u2010forming pathway. Here, we present a strategy that combines a molecular additive, tris(4\u2010fluorophenyl)phosphine (TFPP), with a tailored formation protocol to mitigate monomer\u2010induced degradation. Prior to oxidative decomposition, TFPP modifies the interfacial environment of NCM through early surface interaction and partial coverage, reducing the accessibility of residual monomers to the cathode interface. The formation protocol then promotes preferential TFPP decomposition before extensive monomer oxidation, enabling a protective CEI with a LiF\u2010rich inner region. This sequential interfacial regulation suppresses monomer\u2010driven side reactions, reduces electrolyte consumption, stabilizes Li\u2010ion transport, and mitigates structural degradation of the cathode. Consequently, a 2 Ah\u2010level pouch cell delivering 303\u00a0Wh kg\n                    <jats:sup>\u22121<\/jats:sup>\n                    retained 82.8% capacity after 150 cycles under lean electrolyte conditions (2\u00a0g Ah\n                    <jats:sup>\u22121<\/jats:sup>\n                    ). This work thus provides a practical strategy for developing more durable high\u2010energy\u2010density GPE\u2010based batteries.\n                  <\/jats:p>","DOI":"10.1002\/anie.1297472","type":"journal-article","created":{"date-parts":[[2026,9,28]],"date-time":"2026-09-28T12:49:43Z","timestamp":1790599783000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Mechanistic Control of Cathode\u2013Electrolyte Interphase Formation in Gel Polymer Electrolyte for Lithium\u2010Ion Batteries"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0000-7285-7845","authenticated-orcid":false,"given":"Sang Goo","family":"Kang","sequence":"first","affiliation":[{"name":"Department of Chemical and Biomolecular Engineering Yonsei University  Seodaemun\u2010gu Seoul Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jeonghyun","family":"Ko","sequence":"additional","affiliation":[{"name":"Next Generation Battery Office SK On  Yuseong\u2010gu Daejeon Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Gunyoung","family":"Kim","sequence":"additional","affiliation":[{"name":"Next Generation Battery Office SK On  Yuseong\u2010gu Daejeon Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9951-1323","authenticated-orcid":false,"given":"Jaehoon","family":"Choi","sequence":"additional","affiliation":[{"name":"Next Generation Battery Office SK On  Yuseong\u2010gu Daejeon Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6629-3147","authenticated-orcid":false,"given":"Jong Hyeok","family":"Park","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biomolecular Engineering Yonsei University  Seodaemun\u2010gu Seoul Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,9,28]]},"reference":[{"key":"e_1_2_9_2_1","doi-asserted-by":"publisher","DOI":"10.1038\/451652a"},{"key":"e_1_2_9_3_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201105006"},{"key":"e_1_2_9_4_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.201800561"},{"key":"e_1_2_9_5_1","doi-asserted-by":"publisher","DOI":"10.1021\/cr030203g"},{"key":"e_1_2_9_6_1","doi-asserted-by":"publisher","DOI":"10.1039\/C8TA08997C"},{"key":"e_1_2_9_7_1","doi-asserted-by":"publisher","DOI":"10.1038\/natrevmats.2016.103"},{"key":"e_1_2_9_8_1","doi-asserted-by":"publisher","DOI":"10.1039\/C7EE00534B"},{"key":"e_1_2_9_9_1","doi-asserted-by":"publisher","DOI":"10.1002\/aenm.201702184"},{"key":"e_1_2_9_10_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ensm.2020.10.018"},{"key":"e_1_2_9_11_1","doi-asserted-by":"publisher","DOI":"10.1039\/D3CS00551H"},{"key":"e_1_2_9_12_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.201804909"},{"key":"e_1_2_9_13_1","doi-asserted-by":"publisher","DOI":"10.1002\/inf2.12232"},{"key":"e_1_2_9_14_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010024\u201049713\u2010z"},{"key":"e_1_2_9_15_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202314063"},{"key":"e_1_2_9_16_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ensm.2019.09.011"},{"key":"e_1_2_9_17_1","doi-asserted-by":"publisher","DOI":"10.1007\/s40820\u2010024\u201001354\u2010z"},{"key":"e_1_2_9_18_1","doi-asserted-by":"publisher","DOI":"10.1002\/eem2.12469"},{"key":"e_1_2_9_19_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2022.139339"},{"key":"e_1_2_9_20_1","doi-asserted-by":"publisher","DOI":"10.1021\/ma9902955"},{"key":"e_1_2_9_21_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202424568"},{"key":"e_1_2_9_22_1","doi-asserted-by":"publisher","DOI":"10.1007\/s40820\u2010022\u201000917\u20102"},{"key":"e_1_2_9_23_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202300057"},{"key":"e_1_2_9_24_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.nanolett.3c01700"},{"key":"e_1_2_9_25_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.nanoen.2020.105282"},{"key":"e_1_2_9_26_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsami.7b08953"},{"key":"e_1_2_9_27_1","article-title":"Implications 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