{"paper_id":"442370b1-355e-4afe-bf94-e8ca4b90858e","body_text":"Cu(FSI)₂-Triggered Interfacial In-Situ Polymerization of DOL for High-Performance Solid-State Lithium Metal Batteries | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Research Article Cu(FSI)₂-Triggered Interfacial In-Situ Polymerization of DOL for High-Performance Solid-State Lithium Metal Batteries Jintian Wu, Zixuan Fang, Lifen Wang This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-8054957/v1 This work is licensed under a CC BY 4.0 License Status: Under Revision Version 1 posted 21 You are reading this latest preprint version Abstract The limited ionic conductivity and unstable interfaces, primarily caused by poor solid–solid contact, pose significant challenges to the stable cycling of solid-state batteries. This study proposes an interfacial in-situ polymerization strategy to construct a poly(1,3-dioxolane) (PDOL) gel electrolyte layer between a poly(vinylidene fluoride) (PVDF)-based solid polymer electrolyte and the electrodes. This approach aims to address interfacial compatibility issues in solid-state lithium metal batteries. By precisely tuning the composition of the gel precursor and employing characterization techniques such as FTIR and NMR, the efficient ring-opening polymerization of DOL was confirmed, achieving a high conversion rate of 90%. The precursor was drop-cast onto the PVDF-based electrolyte/electrode interfaces before cell assembly. Electrochemical evaluations revealed that the in-situ formed solidified interlayer significantly enhanced interfacial compatibility and ion transport, yielding a high Li⁺ transference number (0.341), an exceptional critical current density (1.4 mA cm⁻²), and remarkable cycling stability exceeding 1600 hours in Li||Li symmetric cells. Furthermore, full cells incorporating LiFePO₄ cathodes demonstrated excellent rate capability and long-term cyclability, retaining 92.1% of their capacity after 1200 cycles. These results collectively underscore the effectiveness of this in-situ solidification strategy in optimizing the interface structure and improving the overall performance of PVDF-based solid-state batteries. PVDF. Ring-opening polymerization. Solid-state battery. DOL Full Text Additional Declarations No competing interests reported. Cite Share Download PDF Status: Under Revision Version 1 posted Editorial decision: Revision requested 27 Nov, 2025 Reviews received at journal 26 Nov, 2025 Reviews received at journal 24 Nov, 2025 Reviews received at journal 22 Nov, 2025 Reviews received at journal 20 Nov, 2025 Reviews received at journal 19 Nov, 2025 Reviews received at journal 16 Nov, 2025 Reviews received at journal 16 Nov, 2025 Reviewers agreed at journal 16 Nov, 2025 Reviewers agreed at journal 14 Nov, 2025 Reviewers agreed at journal 14 Nov, 2025 Reviewers agreed at journal 13 Nov, 2025 Reviewers agreed at journal 13 Nov, 2025 Reviews received at journal 13 Nov, 2025 Reviewers agreed at journal 12 Nov, 2025 Reviewers agreed at journal 12 Nov, 2025 Reviewers agreed at journal 12 Nov, 2025 Reviewers invited by journal 12 Nov, 2025 Editor assigned by journal 11 Nov, 2025 Submission checks completed at journal 11 Nov, 2025 First submitted to journal 07 Nov, 2025 You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. 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Solid-State Lithium Metal Batteries\",\"fulltext\":[],\"fulltextSource\":\"\",\"fullText\":\"\",\"funders\":[],\"hasAdminPriorityOnWorkflow\":false,\"hasManuscriptDocX\":false,\"hasOptedInToPreprint\":true,\"hasPassedJournalQc\":\"\",\"hasAnyPriority\":false,\"hideJournal\":false,\"highlight\":\"\",\"institution\":\"\",\"isAcceptedByJournal\":false,\"isAuthorSuppliedPdf\":true,\"isDeskRejected\":\"\",\"isHiddenFromSearch\":false,\"isInQc\":false,\"isInWorkflow\":false,\"isPdf\":true,\"isPdfUpToDate\":true,\"isWithdrawnOrRetracted\":false,\"journal\":{\"display\":true,\"email\":\"info@researchsquare.com\",\"identity\":\"ionics\",\"isNatureJournal\":false,\"hasQc\":true,\"allowDirectSubmit\":false,\"externalIdentity\":\"\",\"sideBox\":\" Learn more about [Ionics](https://www.springer.com/journal/11581) \",\"snPcode\":\"11581\",\"submissionUrl\":\"https://mc.manuscriptcentral.com/ionics\",\"title\":\"Ionics\",\"twitterHandle\":\"\",\"acdcEnabled\":true,\"dfaEnabled\":true,\"editorialSystem\":\"stoa\",\"reportingPortfolio\":\"Springer Hybrid\",\"inReviewEnabled\":true,\"inReviewRevisionsEnabled\":false},\"keywords\":\"PVDF. Ring-opening polymerization. Solid-state battery. DOL\",\"lastPublishedDoi\":\"10.21203/rs.3.rs-8054957/v1\",\"lastPublishedDoiUrl\":\"https://doi.org/10.21203/rs.3.rs-8054957/v1\",\"license\":{\"name\":\"CC BY 4.0\",\"url\":\"https://creativecommons.org/licenses/by/4.0/\"},\"manuscriptAbstract\":\"\\u003cp\\u003eThe limited ionic conductivity and unstable interfaces, primarily caused by poor solid\\u0026ndash;solid contact, pose significant challenges to the stable cycling of solid-state batteries. This study proposes an interfacial in-situ polymerization strategy to construct a poly(1,3-dioxolane) (PDOL) gel electrolyte layer between a poly(vinylidene fluoride) (PVDF)-based solid polymer electrolyte and the electrodes. This approach aims to address interfacial compatibility issues in solid-state lithium metal batteries. By precisely tuning the composition of the gel precursor and employing characterization techniques such as FTIR and NMR, the efficient ring-opening polymerization of DOL was confirmed, achieving a high conversion rate of 90%. The precursor was drop-cast onto the PVDF-based electrolyte/electrode interfaces before cell assembly. Electrochemical evaluations revealed that the in-situ formed solidified interlayer significantly enhanced interfacial compatibility and ion transport, yielding a high Li⁺ transference number (0.341), an exceptional critical current density (1.4 mA cm⁻\\u0026sup2;), and remarkable cycling stability exceeding 1600 hours in Li||Li symmetric cells. Furthermore, full cells incorporating LiFePO₄ cathodes demonstrated excellent rate capability and long-term cyclability, retaining 92.1% of their capacity after 1200 cycles. These results collectively underscore the effectiveness of this in-situ solidification strategy in optimizing the interface structure and improving the overall performance of PVDF-based solid-state batteries.\\u003c/p\\u003e\",\"manuscriptTitle\":\"Cu(FSI)₂-Triggered Interfacial In-Situ Polymerization of DOL for High-Performance Solid-State Lithium Metal Batteries\",\"msid\":\"\",\"msnumber\":\"\",\"nonDraftVersions\":[{\"code\":1,\"date\":\"2025-11-24 18:40:18\",\"doi\":\"10.21203/rs.3.rs-8054957/v1\",\"editorialEvents\":[{\"type\":\"communityComments\",\"content\":0},{\"type\":\"decision\",\"content\":\"Revision 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