Root and suppression of shuttling gain a uniform Li2O interphase toward 610 Wh kg−1 lithium–sulfur 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 Root and suppression of shuttling gain a uniform Li 2 O interphase toward 610 Wh kg −1 lithium–sulfur batteries Shenglin Xiong, Yu Wang, Tianyu Jiang, Peng Wang, Ruohong Ke, and 6 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-8710340/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 Concentration-gradient-driven polysulfide (LiPS) shuttling has long limited lithium–sulfur batteries, whereas the electromigration shuttling pathway induced by ionized LiPS has remained undetected. By combining mass conservation with Faraday’s law, we derive a LiPS conservation equation that quantitatively decouples concentration-gradient and electromigration shuttling, identifying electromigration as a degradation pathway that is strongly enhanced under high current densities. Accordingly, we propose a lithium-reservoir strategy using Ti3C2Tx materials selected through screening to accelerate Li⁺ transport, effectively suppressing electromigration shuttling. Cryo-electron microscopy reveals that the surface chemistry of Ti3C2Tx drives a superoxide radical-mediated formation of a dense and uniform Li2O solid-electrolyte-interphase (SEI), which serves as a robust barrier against residual shuttling. The assembled 9 Ah pouch cells exhibit benchmark energy densities of 611.5 Wh kgtotal⁻1 for 150 cycles. Our study systematically elucidates the root of polysulfide shuttling and introduces a radical-enabled strategy to construct a uniform Li2O SEI, representing a significant advance for battery research. Physical sciences/Chemistry/Electrochemistry/Batteries Physical sciences/Chemistry/Physical chemistry/Chemical physics Full Text Additional Declarations There is NO Competing Interest. Supplementary Files SupplementaryMaterials.pdf Root and suppression of shuttling gain a uniform Li2O interphase toward 610 Wh kg−1 lithium–sulfur batteries 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. 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