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Herein, we report a scalable 19 \u03bcm composite electrolyte based on a porous PTFE scaffold, a PEO\/LiTFSI matrix, and LiClO\n                    <jats:sub>4<\/jats:sub>\n                    \u2010associated UiO\u201066\u2010NH\n                    <jats:sub>2<\/jats:sub>\n                    as a functional filler. In this metal\u2013organic framework (MOF)\u2010assisted dual\u2010salt regulation strategy, LiTFSI is dispersed in the polymer matrix, while LiClO\n                    <jats:sub>4<\/jats:sub>\n                    is pre\u2010associated with the amino\u2010functionalized UiO\u201066 to regulate the local Li\n                    <jats:sup>+<\/jats:sup>\n                    environment. The synergistic effects of the MOF filler and dual salts reduce PEO crystallinity and promote more efficient Li\n                    <jats:sup>+<\/jats:sup>\n                    transport. The porous PTFE scaffold further enables membrane thinning and mechanical reinforcement. As a result, the electrolyte exhibits an ionic conductivity of 2.19\u2009\u00d7\u200910\n                    <jats:sup>\u22124<\/jats:sup>\n                    \u2009S\u2009cm\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 60\u2009\u00b0C, an electrochemical stability window of 4.6\u2009V, a Li\n                    <jats:sup>+<\/jats:sup>\n                    transference number () of 0.69, and a tensile strength of 70\u2009MPa. LiFePO\n                    <jats:sub>4<\/jats:sub>\n                    cells deliver stable cycling with 97% capacity retention after 160 cycles, and good rate capability and compatibility with high\u2010voltage NCM523 cathodes are also demonstrated. This work provides a practical MOF\u2010assisted ion\u2010regulation strategy for designing ultrathin and mechanically robust polymer electrolytes for advanced solid\u2010state batteries.\n                  <\/jats:p>","DOI":"10.1002\/cssc.71126","type":"journal-article","created":{"date-parts":[[2026,9,30]],"date-time":"2026-09-30T04:06:47Z","timestamp":1790741207000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Ultrathin PTFE\u2010Supported Composite Polymer Electrolyte Enabled by Metal\u2013Organic Framework\u2010Assisted Dual\u2010Salt Regulation for Solid\u2010State Lithium Metal Batteries"],"prefix":"10.1002","volume":"19","author":[{"given":"Dehua","family":"Wang","sequence":"first","affiliation":[{"name":"School of Chemical and Environmental Engineering Wuhan Polytechnic University  Wuhan China"},{"name":"Ministry of Education Key Laboratory for the Green Preparation and Application of Functional Materials Hubei Key Laboratory of Polymer Materials School of Materials Science and Engineering Hubei University  Wuhan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenhao","family":"Pan","sequence":"additional","affiliation":[{"name":"Ministry of Education Key Laboratory for the Green Preparation and Application of Functional Materials Hubei Key Laboratory of Polymer Materials School of Materials Science and Engineering Hubei University  Wuhan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaoli","family":"Chen","sequence":"additional","affiliation":[{"name":"School of Chemical and Environmental Engineering Wuhan Polytechnic University  Wuhan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mi","family":"Tang","sequence":"additional","affiliation":[{"name":"Ministry of Education Key Laboratory for the Green Preparation and Application of Functional Materials Hubei Key Laboratory of Polymer Materials School of 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