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This study presents a Li+ solvation structure in which hetero strongly solvating solvents are colocalized within the first solvation sheath. This structure was realized using nonfluorinated polar solvents, particularly ethylene carbonate (EC) and sulfolane (SL). In conventional electrolytes, solvent\u2013solvent interactions are typically negligible during solvation, as the coordination environment is dominated by individual Li+\u2013solvent binding energy. In contrast, our system revealed that EC and SL exhibit significant intermolecular interactions even within the solvation shell, forming a structurally cooperative solvation environment. This configuration, driving strong solvent\u2013solvent interactions to effectively weaken Li+\u2013solvent interactions, facilitated two critical processes: (1) enhanced Li+ desolvation, enabling more efficient lithium metal deposition, and (2) anion incorporation into the first solvation sheath, stabilizing the solid-electrolyte interphase (SEI). As a result, the optimized electrolyte based on dual strong solvents achieved high lithium metal reversibility (initially 98.24%, 99.35% on average for Coulombic efficiency), enabled stable cycling of lithium metal batteries with high-loading cathodes, and suppressed gas evolution and transition metal dissolution under high-voltage operation.<\/jats:p>","DOI":"10.1021\/acsnano.6c02221","type":"journal-article","created":{"date-parts":[[2026,8,4]],"date-time":"2026-08-04T13:13:28Z","timestamp":1785849208000},"page":"21657-21672","source":"Crossref","is-referenced-by-count":0,"title":["Cooperative\nSolvation of Lithium Ion by Dual Strongly-Solvating\nSolvents for Reversible Lithium Metal Batteries"],"prefix":"10.1021","volume":"20","author":[{"given":"Jinki","family":"Hong","sequence":"first","affiliation":[{"name":"Ulsan National Institute of Science and Technology (UNIST) , , 1 00 Banyeon-ri, Eonyang-eup , Ulju-gun, ,","place":["Ulsan, Korea, 44919"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Do Sol","family":"Cheong","sequence":"additional","affiliation":[{"name":"Ulsan National Institute of Science and Technology (UNIST) , , 1 00 Banyeon-ri, Eonyang-eup , Ulju-gun, ,","place":["Ulsan, Korea, 44919"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Minjun","family":"Kwon","sequence":"additional","affiliation":[{"name":"Korea Advanced Institute of Science and Technology (KAIST) , , 291 Daehak-ro , ,","place":["Daejeon, Korea, 34141"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ryeo Yun","family":"Hwang","sequence":"additional","affiliation":[{"name":"LG Energy Solution, Ltd. , , 188, Munji-ro , Yuseong-gu, ,","place":["Daejeon, Korea, 34122"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jihong","family":"Jeong","sequence":"additional","affiliation":[{"name":"Ulsan National Institute of Science and Technology (UNIST) , , 1 00 Banyeon-ri, Eonyang-eup , Ulju-gun, ,","place":["Ulsan, Korea, 44919"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Subin","family":"Lee","sequence":"additional","affiliation":[{"name":"Ulsan National Institute of Science and Technology (UNIST) , , 1 00 Banyeon-ri, Eonyang-eup , Ulju-gun, ,","place":["Ulsan, Korea, 44919"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jeongin","family":"Lee","sequence":"additional","affiliation":[{"name":"Ulsan National Institute of Science and Technology (UNIST) , , 1 00 Banyeon-ri, Eonyang-eup , Ulju-gun, ,","place":["Ulsan, Korea, 44919"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7200-7186","authenticated-orcid":true,"given":"Dong-Hwa","family":"Seo","sequence":"additional","affiliation":[{"name":"Korea Advanced Institute of Science and Technology (KAIST) , , 291 Daehak-ro , ,","place":["Daejeon, Korea, 34141"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7914-4186","authenticated-orcid":true,"given":"Hyun-Kon","family":"Song","sequence":"additional","affiliation":[{"name":"Ulsan National Institute of Science and Technology (UNIST) , , 1 00 Banyeon-ri, Eonyang-eup , Ulju-gun, ,","place":["Ulsan, Korea, 44919"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,28]]},"reference":[{"issue":"7","key":"2026081111122414100_cit1","doi-asserted-by":"publisher","first-page":"1584","DOI":"10.1021\/acsenergylett.9b00822","article-title":"Molecular-Scale\nInterfacial Model for Predicting Electrode Performance in Rechargeable\nBatteries","volume":"4","author":"Ming","year":"2019","journal-title":"ACS Energy Lett."},{"issue":"10","key":"2026081111122414100_cit2","doi-asserted-by":"publisher","first-page":"3040","DOI":"10.1039\/C9CS00838A","article-title":"Towards practical\nlithium-metal anodes","volume":"49","author":"Zhang","year":"2020","journal-title":"Chem. 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