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However, the liquid phase and the polymer matrix act as reciprocal chokes: the liquid expedites ion transport but plasticizes the matrix and compromises its mechanical strength, whereas the matrix provides rigidity yet obstructs ionic conduction. In this study, we propose a molecular scaffold strap strategy that decouples the regulation of mechanical robustness and ion transport in GPEs. Specifically, six\u2010arm monomers are employed to form a 3D polymer matrix, while ethylene glycol dibutyl ether, with a size\u2010matched anchoring character, acts as a scaffold strap that strengthens adjacent polymer segments. Fluorinated carbonate cosolvents further facilitate Li\n                    <jats:sup>+<\/jats:sup>\n                    transport and interfacial stability. The engineered GPE exhibits a high modulus of 8.9\u00a0MPa, ionic conductivity of 3.82 \u00d7 10\n                    <jats:sup>\u22124<\/jats:sup>\n                    S cm\n                    <jats:sup>\u22121<\/jats:sup>\n                    , Li\n                    <jats:sup>+<\/jats:sup>\n                    transference number of 0.68, and stable electrode interfaces. The Li||LiNi\n                    <jats:sub>0.8<\/jats:sub>\n                    Co\n                    <jats:sub>0.1<\/jats:sub>\n                    Mn\n                    <jats:sub>0.1<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    pouch cell (2.7 Ah) achieves 87% capacity retention after 100 cycles and exhibits an elevated self\u2010heating onset temperature of 160.7\u00b0C. Furthermore, a high energy density of 506\u00a0Wh kg\n                    <jats:sup>\u22121<\/jats:sup>\n                    is demonstrated in the Cu||LiNi\n                    <jats:sub>0.92<\/jats:sub>\n                    Co\n                    <jats:sub>0.03<\/jats:sub>\n                    Mn\n                    <jats:sub>0.05<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    pouch cell (3.5 Ah).\n                  <\/jats:p>","DOI":"10.1002\/anie.3049996","type":"journal-article","created":{"date-parts":[[2026,9,9]],"date-time":"2026-09-09T04:13:33Z","timestamp":1788927213000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Spatially Decoupled Ion Transport and Mechanical Robustness Enabled by a Molecular Scaffold Strap in Gel Polymer Electrolytes"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-8637-3590","authenticated-orcid":false,"given":"Xin","family":"Shen","sequence":"first","affiliation":[{"name":"Z Energy Storage Center Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education School of Energy and Environment Southeast University  Nanjing Jiangsu P. 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