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Poly(1,3\u2010dioxane) (PDOL)\u2010based electrolytes have attracted significant attention due to the pseudo\u2010high conductivity achieved through sophisticated in situ polymerization methods; however, such PDOL\u2010based electrolytes present challenges of crystallization over time and monomers residual during processing. In this study, integrating LiTFSI and LiDFOB as a universal copolymerization strategy for developing high\u2010performance PDOL electrolytes with a wide range of epoxy crosslinkers is proposed. It is discovered that this approach leverages the protective effects of TFSI anions on the boron active center and catalyzes polymer chain growth via crosslinking. The homogenously crosslinked (benzene\u2010centered) PDOL electrolyte exhibits remarkable thermo\u2010mechanical stability (up to 100\u00a0\u00b0C), high ion migration number (\n                    <jats:italic>t<\/jats:italic>\n                    <jats:sub>Li+<\/jats:sub>\n                    = 0.42), a wide electrochemical window (\u22485.0\u00a0V vs Li\n                    <jats:sup>+<\/jats:sup>\n                    \/Li), and high ionic conductivity (4.5\u00d710\n                    <jats:sup>\u22124<\/jats:sup>\n                    S cm\n                    <jats:sup>\u22121<\/jats:sup>\n                    ). Notably, the crosslinked PDOL electrolyte is in the all\u2010solid\u2010state with minimal monomer\/oligomer residual, exhibiting no crystallization during relaxation, delivering a robust performance in all\u2010solid\u2010state lithium metal batteries.\n                  <\/jats:p>","DOI":"10.1002\/advs.202405482","type":"journal-article","created":{"date-parts":[[2024,7,29]],"date-time":"2024-07-29T07:20:37Z","timestamp":1722237637000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":40,"title":["Universal Copolymerization of Crosslinked Polyether Electrolytes for All\u2010Solid\u2010State Lithium\u2010Metal Batteries"],"prefix":"10.1002","volume":"11","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-5090-5543","authenticated-orcid":false,"given":"Chengjun","family":"Lei","sequence":"first","affiliation":[{"name":"State Key Laboratory of Chem\/Bio\u2010Sensing and Chemometrics, Joint International Research Laboratory of Energy Electrochemistry, College of Chemistry and Chemical Engineering Hunan University  Changsha 410082 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tiankun","family":"Zhou","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chem\/Bio\u2010Sensing and Chemometrics, Joint International Research Laboratory of Energy Electrochemistry, College of Chemistry and Chemical Engineering Hunan University  Changsha 410082 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mingjie","family":"Zhang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chem\/Bio\u2010Sensing and Chemometrics, Joint International Research Laboratory of Energy Electrochemistry, College of Chemistry and Chemical Engineering Hunan University  Changsha 410082 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tingting","family":"Liu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chem\/Bio\u2010Sensing and Chemometrics, Joint International Research Laboratory of Energy Electrochemistry, College of Chemistry and Chemical Engineering Hunan University  Changsha 410082 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chen","family":"Xu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chem\/Bio\u2010Sensing and Chemometrics, Joint International Research Laboratory of Energy Electrochemistry, College of Chemistry and Chemical Engineering Hunan University  Changsha 410082 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rui","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chem\/Bio\u2010Sensing and Chemometrics, Joint International Research Laboratory of Energy Electrochemistry, College of Chemistry and Chemical Engineering Hunan University  Changsha 410082 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xin","family":"He","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chem\/Bio\u2010Sensing and Chemometrics, Joint International Research Laboratory of Energy Electrochemistry, College of Chemistry and Chemical Engineering Hunan University  Changsha 410082 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4074-340X","authenticated-orcid":false,"given":"Xiao","family":"Liang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chem\/Bio\u2010Sensing and Chemometrics, Joint International Research Laboratory of Energy Electrochemistry, College of Chemistry and Chemical Engineering Hunan University  Changsha 410082 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2024,7,29]]},"reference":[{"key":"e_1_2_8_1_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41563-023-01693-z"},{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202004793"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-023-40394-8"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1002\/ese3.1163"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1002\/batt.202200502"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-022-31792-5"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsami.2c17581"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41560-019-0349-7"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.mtphys.2022.100620"},{"key":"e_1_2_8_10_1","first-page":"2708","volume":"14","author":"Vijayakumar V.","year":"2021","journal-title":"Environ. 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