Non-Arrhenius Li-ion transport and grain-size effects in argyrodite solid electrolytes

Non-Arrhenius Li-ion transport and grain-size effects in argyrodite solid electrolytes | 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 Non-Arrhenius Li-ion transport and grain-size effects in argyrodite solid electrolytes Yongliang Ou, Lena Scholz, Sanath Keshav, Yuji Ikeda, Marvin Kraft, and 5 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7913719/v1 This work is licensed under a CC BY 4.0 License Status: Under Review Version 1 posted You are reading this latest preprint version Abstract Argyrodite solid electrolytes, such as Li$_6$PS$_5$Cl, exhibit some of the highest known superionic conductivities. Yet, the mechanistic understanding of Li$^+$ transport in realistic argyrodite microstructures---where atomic-scale mechanisms interplay with continuum-scale dynamics at grain boundaries---remains limited. Here, we resolve Li$^+$ transport in silico by developing accurate machine-learning potentials via closed-loop active learning and embedding the potentials in a multiscale modeling framework that integrates molecular dynamics with finite element simulations. We show that bulk diffusion barriers scale linearly with anion radius. Grain boundaries have opposite effects depending on the bulk---enhancing Li$^+$ diffusion in low-diffusivity phases but suppressing it in fast-diffusing ones. Simulations of polycrystalline Li$_6$PS$_5$I reveal non-Arrhenius transport behaviors consistent with experiments. Grain-size-dependent predictions indicate that grain refinement improves intergranular contacts in argyrodites without compromising superionic conductivity, while nanosizing can activate ionic transport in electrolytes lacking intrinsic superionic behavior. Our findings highlight the decisive role of microstructure in developing solid electrolytes. Physical sciences/Materials science/Materials for energy and catalysis/Batteries Physical sciences/Materials science/Theory and computation/Atomistic models Physical sciences/Chemistry/Theoretical chemistry/Molecular dynamics Full Text Additional Declarations There is NO Competing Interest. Supplementary Files SIlocalactivelearning.pdf Supplementary information for: Non-Arrhenius Li-ion transport and grain-size effects in argyrodite solid electrolytes Cite Share Download PDF Status: Under Review 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-7913719","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":546323916,"identity":"f380886b-4299-49b9-a137-60e560f29c48","order_by":0,"name":"Yongliang 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