Current-Driven SEI and Near-Surface Structural and Chemical Evolution in Lithium Metal Batteries

Current-Driven SEI and Near-Surface Structural and Chemical Evolution in Lithium Metal 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 Current-Driven SEI and Near-Surface Structural and Chemical Evolution in Lithium Metal Batteries Henrique D. Minami, Francisco A. Ospina Acevedo, Jorge M. Seminario, and 1 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-8264591/v1 This work is licensed under a CC BY 4.0 License Status: Under Revision Version 1 posted 14 You are reading this latest preprint version Abstract Lithium metal batteries promise of exceptional energy density is hindered by unstable solid electrolyte interphases (SEIs), which are highly sensitive to electrolyte composition and operating current. While weakly solvating and localized high-concentration electrolytes (LHCE) have shown potential to stabilize the SEI, the influence of current density on SEI evolution remains insufficiently understood. In this work, we integrate a Hybrid Ab Initio Reactive (HAIR) atomistic simulation method for generating realistic SEI structures with a novel Ionic-Current–Electric-Field (ICEF) framework to predict current-dependent ion transport using ReaxFF molecular dynamics. We apply this approach to two ether-based LHCE electrolytes, with chemistry differing only by addition of a small amount of a weak solvent to one of them, but marked differences in solvation structures, SEI structure and morphologies, and interactions with incoming ions. Our simulations reveal that elevated current densities destabilize some SEI components and stabilize others, forming specific aggregate species in the near-surface layer for each type of electrolytes, and inducing asymmetric Li⁺ desolvation, potentially affecting lithium deposition morphology and Coulombic efficiency. These findings demonstrate a clear dependence of SEI and near-surface layer composition and stability on current density, underscoring the importance of current as a critical design parameter. This framework offers a pathway for rational electrolyte engineering aimed at achieving stable, high-rate lithium metal batteries. Physical sciences/Chemistry Physical sciences/Energy science and technology Physical sciences/Materials science Full Text Additional Declarations No competing interests reported. Supplementary Files DF2M47SI.docx Cite Share Download PDF Status: Under Revision Version 1 posted Editorial decision: Revision requested 06 Mar, 2026 Reviews received at journal 16 Feb, 2026 Reviewers agreed at journal 13 Feb, 2026 Reviewers agreed at journal 12 Feb, 2026 Reviews received at journal 04 Feb, 2026 Reviewers agreed at journal 02 Feb, 2026 Reviewers agreed at journal 30 Jan, 2026 Reviews received at journal 20 Jan, 2026 Reviewers agreed at journal 28 Dec, 2025 Reviewers agreed at journal 28 Dec, 2025 Reviewers invited by journal 22 Dec, 2025 Editor assigned by journal 07 Dec, 2025 Submission checks completed at journal 05 Dec, 2025 First submitted to journal 02 Dec, 2025 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-8264591","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":564111628,"identity":"9e60064e-2aa8-4f48-99d4-d86d6cfb928f","order_by":0,"name":"Henrique D. 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While weakly solvating and localized high-concentration electrolytes (LHCE) have shown potential to stabilize the SEI, the influence of current density on SEI evolution remains insufficiently understood. In this work, we integrate a Hybrid Ab Initio Reactive (HAIR) atomistic simulation method for generating realistic SEI structures with a novel Ionic-Current\u0026ndash;Electric-Field (ICEF) framework to predict current-dependent ion transport using ReaxFF molecular dynamics. We apply this approach to two ether-based LHCE electrolytes, with chemistry differing only by addition of a small amount of a weak solvent to one of them, but marked differences in solvation structures, SEI structure and morphologies, and interactions with incoming ions. Our simulations reveal that elevated current densities destabilize some SEI components and stabilize others, forming specific aggregate species in the near-surface layer for each type of electrolytes, and inducing asymmetric Li⁺ desolvation, potentially affecting lithium deposition morphology and Coulombic efficiency. These findings demonstrate a clear dependence of SEI and near-surface layer composition and stability on current density, underscoring the importance of current as a critical design parameter. This framework offers a pathway for rational electrolyte engineering aimed at achieving stable, high-rate lithium metal batteries.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e","manuscriptTitle":"Current-Driven SEI and Near-Surface Structural and Chemical Evolution in Lithium Metal Batteries","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2025-12-24 10:46:38","doi":"10.21203/rs.3.rs-8264591/v1","editorialEvents":[{"type":"communityComments","content":0},{"type":"decision","content":"Revision requested","date":"2026-03-06T15:06:29+00:00","index":"","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2026-02-16T22:00:38+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"328899974983658974215044321701100802942","date":"2026-02-13T10:58:48+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"206552802924273231351016599988446246895","date":"2026-02-12T19:15:29+00:00","index":"hide","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2026-02-05T00:35:55+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"261342471398153040341131652489793635152","date":"2026-02-02T15:16:57+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"93048690965183839861442033959521387212","date":"2026-01-30T05:40:34+00:00","index":"hide","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2026-01-20T13:14:59+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"127450264947312657136358889817540793290","date":"2025-12-29T01:05:49+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"3323258079867410583460854067157335745","date":"2025-12-28T18:59:45+00:00","index":"hide","fulltext":""},{"type":"reviewersInvited","content":"","date":"2025-12-22T12:00:36+00:00","index":"","fulltext":""},{"type":"editorAssigned","content":"","date":"2025-12-07T12:37:49+00:00","index":"","fulltext":""},{"type":"checksComplete","content":"","date":"2025-12-05T19:56:51+00:00","index":"","fulltext":""},{"type":"submitted","content":"npj Energy Materials","date":"2025-12-03T00:15:24+00:00","index":"","fulltext":""}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"npj-energy-materials","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"","sideBox":"Learn more about [npj Energy Materials](https://www.nature.com/npjenergymats/)","snPcode":"44456","submissionUrl":"https://submission.springernature.com/new-submission/44456/3","title":"npj Energy Materials","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"stoa","reportingPortfolio":"Unsupported Journal","inReviewEnabled":true,"inReviewRevisionsEnabled":true}}],"origin":"","ownerIdentity":"eaac7c72-b796-48e9-b092-55ba290addfe","owner":[],"postedDate":"December 24th, 2025","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"in-revision","subjectAreas":[{"id":60065604,"name":"Physical sciences/Chemistry"},{"id":60065605,"name":"Physical sciences/Energy science and technology"},{"id":60065606,"name":"Physical sciences/Materials science"}],"tags":[],"updatedAt":"2026-03-06T15:09:43+00:00","versionOfRecord":[],"versionCreatedAt":"2025-12-24 10:46:38","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-8264591","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-8264591","identity":"rs-8264591","version":["v1"]},"buildId":"8U1c8b4HqxoKbykW_rLl7","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}