A machine-learned superionic, Li-metal-compatible, and cost-effective halide electrolyte for all-solid-state Li metal batteries

A machine-learned superionic, Li-metal-compatible, and cost-effective halide electrolyte for all-solid-state Li 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 Article A machine-learned superionic, Li-metal-compatible, and cost-effective halide electrolyte for all-solid-state Li metal batteries Ce-Wen Nan, Hong Liu, haoyu yin, Xiang Qi, Yaoyu Ren, Meng Wu, and 12 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-8526688/v1 This work is licensed under a CC BY 4.0 License Status: Posted Version 1 posted You are reading this latest preprint version Abstract Halide solid electrolytes are promising for high-voltage cathodes, yet a combination of high ionic conductivity, robust Li metal compatibility, and cost-effectiveness, is fundamentally challenging to achieve. Here, assisted by a generative machine learning approach, we identify a Ti/F co-doping strategy in the cost-effective Li2ZrCl6 system to improve both ionic conductivity and Li metal compatibility. Substituting Zr with the more electronegative Ti induces a powerful inductive effect to weaken Li+-anion coupling, thereby significantly reducing the a-b plane migration barrier and transforming the native 1D ionic transport into a 3D percolating network. The resulting electrolyte, Li2.1Zr0.9Ti0.1Cl5.7F0.3, achieves a room-temperature ionic conductivity of 2.9 mS cm⁻1 and robust Li metal compatibility with long-term cycling stability exceeding 2000 h at 1 mA cm⁻2 in Li symmetric cells. Moreover, the electrolyte exhibits remarkable air stability under dry-room condition and significantly low materials cost, validating its great potential for large-scale production. This unique combination of high ionic conductivity and robust Li metal compatibility enables the all-solid-state Li metal batteries with uncoated LiNi0.8Mn0.1Co0.1O2 cathode to realize stable cycling performance (86.5% capacity retention after 1000 cycles at 1 C in mold-type cells) and high areal capacity (3.6 mAh cm⁻2 in pouch-type cells), demonstrating a viable path towards practical, high-energy-density devices. This work establishes a new paradigm for rapidly and efficiently screening key target materials for practical device applications. Physical sciences/Chemistry/Electrochemistry/Batteries Physical sciences/Materials science/Materials for energy and catalysis/Batteries Full Text Additional Declarations There is NO Competing Interest. Supplementary Files SupplementarymaterialsforMLelectrolyteLiu.docx Supplementary materials Cite Share Download PDF Status: Posted Version 1 posted 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. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. We do this by developing innovative software and high quality services for the global research community. Our growing team is made up of researchers and industry professionals working together to solve the most critical problems facing scientific publishing. Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-8526688","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":589126962,"identity":"30850a2b-9e43-4d07-82bd-5fb702da0839","order_by":0,"name":"Ce-Wen 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Here, assisted by a generative machine learning approach, we identify a Ti/F co-doping strategy in the cost-effective Li2ZrCl6 system to improve both ionic conductivity and Li metal compatibility. Substituting Zr with the more electronegative Ti induces a powerful inductive effect to weaken Li+-anion coupling, thereby significantly reducing the a-b plane migration barrier and transforming the native 1D ionic transport into a 3D percolating network. The resulting electrolyte, Li2.1Zr0.9Ti0.1Cl5.7F0.3, achieves a room-temperature ionic conductivity of 2.9 mS cm⁻1 and robust Li metal compatibility with long-term cycling stability exceeding 2000 h at 1 mA cm⁻2 in Li symmetric cells. Moreover, the electrolyte exhibits remarkable air stability under dry-room condition and significantly low materials cost, validating its great potential for large-scale production. 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