Breaking the Rate-Limiting Barrier in Solid-Solid Sulfur Redox Reactions via Spin-State Engineering

Breaking the Rate-Limiting Barrier in Solid-Solid Sulfur Redox Reactions via Spin-State Engineering | 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 Breaking the Rate-Limiting Barrier in Solid-Solid Sulfur Redox Reactions via Spin-State Engineering Kwun Nam Hui, Qingbin Jiang, Huifang Xu, Xinyu Ye, Lingwen Liu, and 12 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7227578/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 Elucidating the mechanisms governing sulfur redox reactions is critical for the development of high-energy-density lithium-sulfur (Li-S) batteries. Despite progress, the kinetics of the solid-solid conversion from Li2S2 to Li2S remain poorly understood. Here we show that spin-state transitions within reaction intermediates are the principal source of the sluggish kinetics. Guided by density functional theory and machine-learning-assisted catalyst screening, we have found a negative correlation between the spin moment of the catalyst and the Gibbs free energy barrier for the Li2S2 to Li2S conversion. Among a series of dual-metal doped catalysts, a Co,Ni-MoS2 catalyst, with its exceptional spin moment, effectively regulates the spin states of the reactants, reducing the high reaction energy barrier associated with spin-state transitions. Therefore, Li-S batteries incorporating with the Co,Ni-MoS2 showed accelerated sulfur conversion, particularly during solid-solid transitions, effectively suppressed polysulfide shuttling, and had excellent electrochemical performance. A prototype Li-S pouch cell achieved a capacity exceeding 13.2 Ah and an energy density of 435 Wh kg-1. These findings show critical insights into the role of spin moments in sulfur conversion, providing a way to design efficient and durable catalysts for Li-S batteries. Physical sciences/Materials science/Materials for energy and catalysis/Batteries Physical sciences/Chemistry/Electrochemistry/Batteries Full Text Additional Declarations There is NO Competing Interest. Supplementary Files SupplementaryInformation.pdf Supplementary Information 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. 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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-7227578","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":500089637,"identity":"3c4eac54-e9a3-49b9-9f65-683f29b6f735","order_by":0,"name":"Kwun Nam 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