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Here, we develop a site\u2010selective anion\u2010cation regulation strategy for argyrodite Li\n                    <jats:sub>6<\/jats:sub>\n                    PS\n                    <jats:sub>5<\/jats:sub>\n                    Cl electrolyte to couple framework stabilization with interphase chemistry, enabling long\u2010term dendrite\u2010suppressed cycling under low stack pressure. Al\n                    <jats:sup>3+<\/jats:sup>\n                    substitution for P\n                    <jats:sup>5+<\/jats:sup>\n                    forms AlS\n                    <jats:sub>4<\/jats:sub>\n                    \u2010related local units and strengthens local Al\u2013S bonding, stabilizing the sulfide framework against redox decomposition. Cl\n                    <jats:sup>\u2212<\/jats:sup>\n                    incorporation into the 4\n                    <jats:italic>a<\/jats:italic>\n                    \/4\n                    <jats:italic>d<\/jats:italic>\n                    anion sublattice promotes Li\n                    <jats:sup>+<\/jats:sup>\n                    transport, delivering a high room\u2010temperature ionic conductivity of 7.22\u00a0mS\u00a0cm\n                    <jats:sup>\u22121<\/jats:sup>\n                    . More importantly, F\/Cl regulation redirects the interfacial decomposition pathway from a Li\n                    <jats:sub>2<\/jats:sub>\n                    S\u2010rich\/LiCl interphase toward a LiF\/LiCl\u2010rich and Li\n                    <jats:sub>2<\/jats:sub>\n                    S\u2010poor passivation layer, with exposed LiF\/LiCl (200) planes that exhibit stronger interfacial adhesion with Li metal. Benefiting from this coupled framework\u2010interphase regulation, Li | LAPSCF\u2010Cl | Li symmetric cells cycle for over 8000\u00a0h at 0.5\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    at 3\u00a0MPa and support stable cycling of both NCM811 and sulfur cathodes paired with Li metal under a relatively low pressure of 30\u00a0MPa.\n                  <\/jats:p>","DOI":"10.1002\/anie.3893843","type":"journal-article","created":{"date-parts":[[2026,10,7]],"date-time":"2026-10-07T10:13:12Z","timestamp":1791367992000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Site\u2010Selective Anion\u2010Cation Regulation of Sulfide Electrolyte Enables Low\u2010Pressure Dendrite\u2010Suppressed All\u2010Solid\u2010State Lithium Metal Batteries"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0009-7556-8219","authenticated-orcid":false,"given":"Xinxin","family":"Zhu","sequence":"first","affiliation":[{"name":"Department of Materials Science and Engineering City University of Hong Kong  Hong Kong P. R. China"},{"name":"College of Chemical and Biological Engineering Zhejiang University  Hangzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xianji","family":"Qiao","sequence":"additional","affiliation":[{"name":"i\u2010Lab, CAS Center for Excellence in Nanoscience, Chinese Academy of Sciences Suzhou Institute of Nano\u2010Tech and Nano\u2010Bionics  Suzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2543-8351","authenticated-orcid":false,"given":"Ning","family":"Qin","sequence":"additional","affiliation":[{"name":"College of Chemical and Biological Engineering Zhejiang University  Hangzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhiheng","family":"Li","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering City University of Hong Kong  Hong Kong P. R. 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