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Here, we report a synergistic design strategy for non\u2010flammable and fluorine electrolyte additive combinations that stabilize high\u2010nickel layered cathodes and enable both high energy density and safety. Through a systematic additive screening and thermodynamic analysis based on Gibbs free energy\u2013derived reduction potentials of P2PFS (4,4'\u2010(propane\u20102,2\u2010diyl) bis (4,1\u2010phenylene) disulfo\u2010 fluoridate)\u00a0and related species, we identified additive interactions that suppress exothermic decomposition of carbonate electrolytes. The optimized electrolyte exhibited near non\u2010flammability, significantly improved cycle retention (83% after 200 cycles at 0.3 C), and enhanced interfacial robustness, as confirmed by XPS and TEM analyses. Moreover, 1 Ah\u2010level Li (Ni\n                    <jats:sub>0<\/jats:sub>\n                    .\n                    <jats:sub>8<\/jats:sub>\n                    Co\n                    <jats:sub>0<\/jats:sub>\n                    .\n                    <jats:sub>1<\/jats:sub>\n                    Mn\n                    <jats:sub>0<\/jats:sub>\n                    .\n                    <jats:sub>1<\/jats:sub>\n                    )O\n                    <jats:sub>2<\/jats:sub>\n                    \u2016graphite full cells demonstrated excellent long\u2010term stability (&gt;700 cycles) and no thermal propagation under nail penetration, validating the intrinsic safety of our formulation. The combined thermodynamic\u2013electrochemical approach provides new insights into designing next\u2010generation electrolytes that harmonize non\u2010flammability, cost\u2010effectiveness, and high\u2010voltage stability for advanced lithium\u2010ion batteries.\n                  <\/jats:p>","DOI":"10.1002\/smll.74256","type":"journal-article","created":{"date-parts":[[2026,6,18]],"date-time":"2026-06-18T10:06:17Z","timestamp":1781777177000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Combined Thermodynamic\u2010Electrochemical Understandings of Non\u2010Flammable Electrolyte for High\u2010Nickel Lithium Batteries"],"prefix":"10.1002","volume":"22","author":[{"given":"Myeong Ju","family":"Lee","sequence":"first","affiliation":[{"name":"Smart Materials Research Section Electronics and Telecommunications Research Institute (ETRI)  Daejeon Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ukseon","family":"Shin","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering Korea Advanced Institute of Science and Technology  Daejeon Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jinseo","family":"Kim","sequence":"additional","affiliation":[{"name":"Department of Chemical Engineering Yeungnam University  Gyeongsan\u2010si Gyeongsangbuk\u2010do Republic of Korea"},{"name":"Department of Smart Mobility Engineering Advanced Institute of Science and Technology Kyungpook National University  Daegu Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chanyoung","family":"Lee","sequence":"additional","affiliation":[{"name":"Department of Smart Mobility Engineering Advanced Institute of Science and Technology Kyungpook National University  Daegu Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Eunbin","family":"Noh","sequence":"additional","affiliation":[{"name":"Department of Smart Mobility Engineering Advanced Institute of Science and Technology Kyungpook National University  Daegu Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4016-7265","authenticated-orcid":false,"given":"Kwang Man","family":"Kim","sequence":"additional","affiliation":[{"name":"Smart Materials Research Section Electronics and Telecommunications Research Institute (ETRI)  Daejeon Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7200-7186","authenticated-orcid":false,"given":"Dong\u2010Hwa","family":"Seo","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering Korea Advanced Institute of Science and Technology  Daejeon Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0003-7480-4765","authenticated-orcid":false,"given":"Jimin","family":"Oh","sequence":"additional","affiliation":[{"name":"Smart Materials Research Section Electronics and Telecommunications Research Institute (ETRI)  Daejeon Republic of Korea"},{"name":"Department of Smart Mobility Engineering Advanced Institute of Science and Technology Kyungpook National University  Daegu Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,6,18]]},"reference":[{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jpowsour.2022.231943"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.est.2023.106792"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jpowsour.2020.228803"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1021\/cr500062v"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1038\/nmat2460"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1039\/C5EE00838G"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.est.2023.107761"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsami.3c02770"},{"key":"e_1_2_8_10_1","doi-asserted-by":"publisher","DOI":"10.1039\/D2TA05854E"},{"key":"e_1_2_8_11_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jpowsour.2018.06.046"},{"key":"e_1_2_8_12_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsami.0c04372"},{"key":"e_1_2_8_13_1","first-page":"356","article-title":"High\u2010Voltage Electrolyte and Interface Design for Mid\u2010Nickel High\u2010Energy Li\u2010Ion Batteries","volume":"1","author":"Tran Y. 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