Aqueous Eutectic Electrolytes Suppress Oxygen and Hydrogen Evolution for Long-Life Zn||MnO2 Dual-Electrode-Free Batteries

Aqueous Eutectic Electrolytes Suppress Oxygen and Hydrogen Evolution for Long-Life Zn||MnO2 Dual-Electrode-Free 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 Aqueous Eutectic Electrolytes Suppress Oxygen and Hydrogen Evolution for Long-Life Zn||MnO 2 Dual-Electrode-Free Batteries Linda Nazar, Jinghan Li, Chang Li, Bo Liu, Yuzhang Li, Oleg Borodin This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-6754750/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 23 Jan, 2026 Read the published version in Nature Energy → Version 1 posted You are reading this latest preprint version Abstract Aqueous Zn 2+ /Zn||MnO 2 /Mn 2+ batteries - operating on electrodeposition/dissolution - offer promising high-voltage, high-capacity grid storage capabilities but require acidic conditions for MnO 2 /Mn 2+ conversion that induces problematic zinc corrosion. Here we present a global approach that identifies deep eutectic aqueous-organic electrolytes that strategically disrupt water's hydrogen bonding network, simultaneously enhancing MnO 2 reversibility at the cathode without OER while enabling stable zinc cycling at the anode without HER. Such non-flammable electrolytes regulate the cation solvation structure and phase of the deposited MnO 2 and its morphology, promoting layered structures with enhanced ion transport pathways that significantly improve stripping efficiency. These deep eutectics increase the oxygen evolution overpotential by 0.6 V, well above the MnO 2 deposition potential, which completely suppresses unwanted O 2 evolution. Moreover, they alter the local environment at the cathode interface to create localized interfacial pH gradients that influence critical processes, including optimizing proton transport and MnO 2 stripping. Our Zn 2+ /Zn||MnO 2 /Mn 2+ dual-electrode-free battery achieves high Coulombic efficiency for extended cycling (>5000 cycles) without external acid addition, advancing high-energy-density zinc-manganese battery development through rational electrolyte design. Physical sciences/Chemistry/Energy Physical sciences/Materials science/Materials for energy and catalysis/Batteries Physical sciences/Chemistry/Electrochemistry/Batteries Physical sciences/Chemistry/Green chemistry/Sustainability Physical sciences/Materials science/Materials for energy and catalysis/Electrochemistry/Batteries Full Text Additional Declarations There is NO Competing Interest. Supplementary Files Eutecticelectrolyteflammabilitytest.mp4 Eutectic electrolyte flammability test ZnMnO2SuppInforevtoNENERGY2.pdf Supplementary Information Cite Share Download PDF Status: Published Journal Publication published 23 Jan, 2026 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. 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-6754750","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":532400454,"identity":"1e394697-49b9-4209-870f-8c5e3d4c49cf","order_by":0,"name":"Linda 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Batteries\u003c/p\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 Portfolio","twitterHandle":"","acdcEnabled":false,"dfaEnabled":false,"editorialSystem":"ejp","reportingPortfolio":"","inReviewEnabled":true,"inReviewRevisionsEnabled":false},"keywords":"","lastPublishedDoi":"10.21203/rs.3.rs-6754750/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-6754750/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eAqueous Zn\u003csup\u003e2+\u003c/sup\u003e/Zn||MnO\u003csub\u003e2\u003c/sub\u003e/Mn\u003csup\u003e2+\u003c/sup\u003e batteries - operating on electrodeposition/dissolution - offer promising high-voltage, high-capacity grid storage capabilities but require acidic conditions for MnO\u003csub\u003e2\u003c/sub\u003e/Mn\u003csup\u003e2+\u003c/sup\u003e conversion that induces problematic zinc corrosion. Here we present a global approach that identifies deep eutectic aqueous-organic electrolytes that strategically disrupt water's hydrogen bonding network, simultaneously enhancing MnO\u003csub\u003e2\u003c/sub\u003e reversibility at the cathode without OER while enabling stable zinc cycling at the anode without HER. Such non-flammable electrolytes regulate the cation solvation structure and phase of the deposited MnO\u003csub\u003e2\u003c/sub\u003e and its morphology, promoting layered structures with enhanced ion transport pathways that significantly improve stripping efficiency. These deep eutectics increase the oxygen evolution overpotential by 0.6 V, well above the MnO\u003csub\u003e2\u003c/sub\u003e deposition potential, which completely suppresses unwanted O\u003csub\u003e2\u003c/sub\u003e evolution. Moreover, they alter the local environment at the cathode interface to create localized interfacial pH gradients that influence critical processes, including optimizing proton transport and MnO\u003csub\u003e2\u003c/sub\u003e stripping. Our Zn\u003csup\u003e2+\u003c/sup\u003e/Zn||MnO\u003csub\u003e2\u003c/sub\u003e/Mn\u003csup\u003e2+\u003c/sup\u003e dual-electrode-free battery achieves high Coulombic efficiency for extended cycling (\u0026gt;5000 cycles) without external acid addition, advancing high-energy-density zinc-manganese battery development through rational electrolyte design.\u003c/p\u003e","manuscriptTitle":"Aqueous Eutectic Electrolytes Suppress Oxygen and Hydrogen Evolution for Long-Life Zn||MnO2 Dual-Electrode-Free Batteries","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2025-10-29 08:22:44","doi":"10.21203/rs.3.rs-6754750/v1","editorialEvents":[],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"nature-energy","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"nenergy","sideBox":"Learn more about [Nature Energy](http://www.nature.com/nenergy/)","snPcode":"","submissionUrl":"","title":"Nature Energy","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"ejp","reportingPortfolio":"Nature Research","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"abcb875d-7d6b-4bb9-88d0-1a092b064b82","owner":[],"postedDate":"October 29th, 2025","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"published-in-journal","subjectAreas":[{"id":57073719,"name":"Physical sciences/Chemistry/Energy"},{"id":57073720,"name":"Physical sciences/Materials science/Materials for energy and catalysis/Batteries"},{"id":57073721,"name":"Physical sciences/Chemistry/Electrochemistry/Batteries"},{"id":57073722,"name":"Physical sciences/Chemistry/Green chemistry/Sustainability"},{"id":57073723,"name":"Physical sciences/Materials science/Materials for energy and catalysis/Electrochemistry/Batteries"}],"tags":[],"updatedAt":"2026-01-27T09:46:09+00:00","versionOfRecord":{"articleIdentity":"rs-6754750","link":"https://doi.org/10.1038/s41560-025-01958-8","journal":{"identity":"nature-energy","isVorOnly":false,"title":"Nature Energy"},"publishedOn":"2026-01-23 05:00:00","publishedOnDateReadable":"January 23rd, 2026"},"versionCreatedAt":"2025-10-29 08:22:44","video":"","vorDoi":"10.1038/s41560-025-01958-8","vorDoiUrl":"https://doi.org/10.1038/s41560-025-01958-8","workflowStages":[]},"version":"v1","identity":"rs-6754750","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-6754750","identity":"rs-6754750","version":["v1"]},"buildId":"8U1c8b4HqxoKbykW_rLl7","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}