Leveraging Entropy for Enhanced Energy Density in Cathode-Active Materials for Li-ion Batteries

Leveraging Entropy for Enhanced Energy Density in Cathode-Active Materials for Li-ion 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 Short Report Leveraging Entropy for Enhanced Energy Density in Cathode-Active Materials for Li-ion Batteries Chae-Ho Yim, Elena A. Baranova, Yaser Abu-Lebdeh This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7623165/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 Cathode-active materials (CAMs) play a crucial role in enhancing the energy density and reducing the cost of Li-ion battery cells. This improvement can be realized in commercially-relevant layered oxides LiNi x Mn y Co z O 2 , known as NMCs, by maximizing the nickel content at the expense of cobalt. While higher nickel content boosts energy density by increasing both potential and capacity, it can result in lower capacity retention compared to first-generation NMC CAMs with x = y = z = 1 or even with z = 1 and x = y = 0. To address this challenge, the high-entropy concept is being explored as a means to improve the material’s structural stability during battery operation, thereby enhancing capacity retention and extending cycle life. This study presents evidence through calculations of the mixing entropy ( ∆S mix = -nR∑xlnx ) effect on CAMs and suggests rational design methods for next-generation CAMs. The mixing entropy is calculated for commercial CAMs and estimated for potential CAMs to achieve better energy density in layered oxide types such as LiNi 0.7 Mn 0.15 Co 0.15 O 2 or LiNi 0.7 Mn 0.25 Al 0.05 O 2 . The findings underscore the potential of 70% nickel and cobalt-free CAMs, utilizing entropy as a design principle. Physical sciences/Energy science and technology Physical sciences/Materials science Physical sciences/Physics Full Text Additional Declarations No competing interests reported. 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-7623165","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Short Report","associatedPublications":[],"authors":[{"id":530208434,"identity":"2615c87c-49ad-4aba-b025-4cd385efb3b4","order_by":0,"name":"Chae-Ho Yim","email":"","orcid":"","institution":"University of Ottawa","correspondingAuthor":false,"prefix":"","firstName":"Chae-Ho","middleName":"","lastName":"Yim","suffix":""},{"id":530208435,"identity":"d8458190-fb46-4c17-a0e7-e9ef9d59404a","order_by":1,"name":"Elena A. 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Batteries\u003c/p\u003e","fulltext":[],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":false,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":true,"highlight":"","institution":"","isAcceptedByJournal":false,"isAuthorSuppliedPdf":true,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":true,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research 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This improvement can be realized in commercially-relevant layered oxides LiNi\u003csub\u003ex\u003c/sub\u003eMn\u003csub\u003ey\u003c/sub\u003eCo\u003csub\u003ez\u003c/sub\u003eO\u003csub\u003e2\u003c/sub\u003e, known as NMCs, by maximizing the nickel content at the expense of cobalt. While higher nickel content boosts energy density by increasing both potential and capacity, it can result in lower capacity retention compared to first-generation NMC CAMs with x\u0026thinsp;=\u0026thinsp;y\u0026thinsp;=\u0026thinsp;z\u0026thinsp;=\u0026thinsp;1 or even with z\u0026thinsp;=\u0026thinsp;1 and x\u0026thinsp;=\u0026thinsp;y\u0026thinsp;=\u0026thinsp;0. To address this challenge, the high-entropy concept is being explored as a means to improve the material\u0026rsquo;s structural stability during battery operation, thereby enhancing capacity retention and extending cycle life. This study presents evidence through calculations of the mixing entropy (\u003cem\u003e∆S\u003c/em\u003e\u003csub\u003e\u003cem\u003emix\u003c/em\u003e\u003c/sub\u003e \u003cem\u003e= -nR\u0026sum;xlnx\u003c/em\u003e) effect on CAMs and suggests rational design methods for next-generation CAMs. The mixing entropy is calculated for commercial CAMs and estimated for potential CAMs to achieve better energy density in layered oxide types such as LiNi\u003csub\u003e0.7\u003c/sub\u003eMn\u003csub\u003e0.15\u003c/sub\u003eCo\u003csub\u003e0.15\u003c/sub\u003eO\u003csub\u003e2\u003c/sub\u003e or LiNi\u003csub\u003e0.7\u003c/sub\u003eMn\u003csub\u003e0.25\u003c/sub\u003eAl\u003csub\u003e0.05\u003c/sub\u003eO\u003csub\u003e2\u003c/sub\u003e. The findings underscore the potential of 70% nickel and cobalt-free CAMs, utilizing entropy as a design principle.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e","manuscriptTitle":"Leveraging Entropy for Enhanced Energy Density in Cathode-Active Materials for Li-ion Batteries","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2025-10-16 05:18:20","doi":"10.21203/rs.3.rs-7623165/v1","editorialEvents":[{"type":"communityComments","content":0}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true}}],"origin":"","ownerIdentity":"ee043d66-1b1f-48e0-944b-b4f0bcd95f26","owner":[],"postedDate":"October 16th, 2025","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"posted","subjectAreas":[{"id":56382830,"name":"Physical sciences/Energy science and technology"},{"id":56382831,"name":"Physical sciences/Materials science"},{"id":56382832,"name":"Physical sciences/Physics"}],"tags":[],"updatedAt":"2025-12-16T22:38:30+00:00","versionOfRecord":[],"versionCreatedAt":"2025-10-16 05:18:20","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-7623165","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-7623165","identity":"rs-7623165","version":["v1"]},"buildId":"XKTyCvWXoU3ODBz1xrDgd","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}