Interfacial Water-Mediated Ion Transport through Electrified Graphene Membranes

Interfacial Water-Mediated Ion Transport through Electrified Graphene Membranes | 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 Interfacial Water-Mediated Ion Transport through Electrified Graphene Membranes Dan Li, Lingzhi Cao, Xiao Wang, Wen-Jie Jiang, Xiaoyang Du, (Jefferson) Zhe Liu This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7453999/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 Ion transport at charged interfaces in aqueous environments is central to a broad spectrum of electrochemical and biological processes1–8. Conventional strategies for electrostatically modulating interfacial ion transport have focused primarily on direct Coulombic interactions, achieved through chemically introduced surface charges9–14 or externally applied potentials15–21, and are typically based on the assumption that water behaves as a passive dielectric medium. Here, we present a nanofluidic platform based on electronically conductive multilayered reduced graphene oxide membranes that reveals a new mechanism of electrically modulated ion transport, in which interfacial water actively governs transport dynamics. This platform enables continuous ion transport measurements across a wide voltage range of both polarities and uncovers strongly asymmetric and nonlinear behaviours, including up to a thousand-fold enhancement in ambipolar diffusivity under strong negative gating, an effect that is unattainable through conventional electrostatics-driven approaches. Molecular dynamics simulations attribute this phenomenon to voltage-induced reorganisation of interfacial water, which promotes ion clustering and fundamentally reshapes interfacial ion dynamics. Our findings establish interfacial water as a voltage-tuneable mediator of ion transport and demonstrate how coupling electrostatic gating with solvent-mediated interactions can enable new designs for electrically responsive nanofluidic and iontronic systems. Physical sciences/Chemistry Physical sciences/Nanoscience and technology Full Text Additional Declarations There is NO Competing Interest. Supplementary Files SupplementaryInformation.pdf Supplementary Information SupplementaryVideo1positivesurfacecharge.mp4 Supplementary Video 1 SupplementaryVideo2negativesurfacecharge.mp4 Supplementary Video 2 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-7453999","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":511712129,"identity":"178cc2c1-46c2-4763-9743-2be7ee7c343e","order_by":0,"name":"Dan 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