Electrochemically-Induced Partial Cation Disorder Eliminates Lattice Collapse in Compositionally-Simple LiNi0.9Mn0.1O2

Electrochemically-Induced Partial Cation Disorder Eliminates Lattice Collapse in Compositionally-Simple LiNi0.9Mn0.1O2 | 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 Physical Sciences - Article Electrochemically-Induced Partial Cation Disorder Eliminates Lattice Collapse in Compositionally-Simple LiNi 0.9 Mn 0.1 O 2 William Chueh, Junghwa Lee, Zhelong Jiang, Nicolas Liang, Howie Nguyen, and 14 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-5284144/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 27 Nov, 2025 Read the published version in Nature Energy → Version 1 posted You are reading this latest preprint version Abstract Virtually all layered oxide positive electrodes (cathodes) for lithium-ion batteries exhibit abrupt shrinkage along the c lattice ( c -collapse) at high states-of-charge, limiting cycle life. In this work, we suppress c -collapse by electrochemically inducing partial disorder permanently throughout the bulk of compositionally-simple LiNi 0.9 Mn 0.1 O 2 . Our approach leverages irreversible oxygen oxidation in the as-synthesized Li-excess Ni-rich oxides to activate partial disordering of the cation sublattice, while preserving the long-range layered structure. Using this method, Li-stoichiometric transition metal oxides with variable extents of cation disorder are readily fabricated by adjusting the starting Li-excess in the as-synthesized materials. Surprisingly, at a TM Li concentration of ≥12%, the c lattice parameter remains nearly invariant during (de)lithiation, leading to decreased chemical strain, enhanced microstructural integrity, and improved battery cycle life. We demonstrate a combination of high specific capacity and long cycle life, along with negligible voltage hysteresis and decay. This concept opens the opportunity for designing materials by inducing persistent intrinsic disorder electrochemically. Physical sciences/Materials science/Materials for energy and catalysis/Batteries Physical sciences/Energy science and technology/Energy storage/Batteries Physical sciences/Materials science/Materials for energy and catalysis/Electrochemistry/Batteries Full Text Additional Declarations There is NO Competing Interest. Supplementary Files LNRSINature.pdf Supplementary Information Cite Share Download PDF Status: Published Journal Publication published 27 Nov, 2025 Read the published version in Nature Energy → 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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LiNi\u003csub\u003e0.9\u003c/sub\u003eMn\u003csub\u003e0.1\u003c/sub\u003eO\u003csub\u003e2\u003c/sub\u003e","fulltext":[],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":false,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":true,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":true,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":true,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"nature-portfolio","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"","title":"Nature 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In this work, we suppress \u003cb\u003ec\u003c/b\u003e-collapse by electrochemically inducing partial disorder permanently throughout the bulk of compositionally-simple LiNi\u003csub\u003e0.9\u003c/sub\u003eMn\u003csub\u003e0.1\u003c/sub\u003eO\u003csub\u003e2\u003c/sub\u003e. Our approach leverages irreversible oxygen oxidation in the as-synthesized Li-excess Ni-rich oxides to activate partial disordering of the cation sublattice, while preserving the long-range layered structure. Using this method, Li-stoichiometric transition metal oxides with variable extents of cation disorder are readily fabricated by adjusting the starting Li-excess in the as-synthesized materials. Surprisingly, at a TM\u003csub\u003eLi\u003c/sub\u003e concentration of ≥12%, the \u003cb\u003ec\u003c/b\u003e lattice parameter remains nearly invariant during (de)lithiation, leading to decreased chemical strain, enhanced microstructural integrity, and improved battery cycle life. We demonstrate a combination of high specific capacity and long cycle life, along with negligible voltage hysteresis and decay. 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