Zinc-oligoether carboxylate salts as electrolyte additives for aqueous Zn metal batteries

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Abstract Aqueous zinc-metal batteries, which pair a water-based electrolyte with an earth-abundant metal, offer an ideal blueprint for sustainable battery technology. However, intrinsic instability owing to hydrogen evolution and dendrite formation during the plating process severely compromise the stability of the Zn anode and drastically limit cycling performance. Extending the battery's lifetime at such a complex interface requires a comprehensive approach promotes the formation of a stable and robust solid electrolyte interphase (SEI) layer. Here, we introduce zinc oligoether carboxylates as tuneable dual-function electrolyte additives. The carboxylate group acts as a proton donor, inducing the decomposition of sulfate salt anions to form a ZnS-based SEI, while the oligoether moiety mitigates water activity at the electrode interface, as deduced from the combination of spectroscopic techniques with scanning electrochemical microscopy. By varying the chain length, we find that the longest chain, Zinc (2-[2-[2-(2-methoxyethoxy)ethoxy]ethoxy]acetate)₂, enables long-term cycling under harsher conditions than previously reported, extending cycle life fivefold, sustaining 1000 hours at low current density and high capacity with excellent CE%. This enhancement translates into 98 mAh Zn-MnO2 full pouch cells, supporting the scalability of commercial Zn-based devices by delivering a promising cycle life at low C-rates and high cumulative charge capacity. We hope this discovery will speed up the development of commercial Zn-MnO2 aqueous batteries.
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Zinc-oligoether carboxylate salts as electrolyte additives for aqueous Zn 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 Zinc-oligoether carboxylate salts as electrolyte additives for aqueous Zn metal batteries Alexis Grimaud, John Brown, Ivette Aguilar, Juan Forero-Saboya, and 6 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7489259/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 20 Dec, 2025 Read the published version in Nature Communications → Version 1 posted You are reading this latest preprint version Abstract Aqueous zinc-metal batteries, which pair a water-based electrolyte with an earth-abundant metal, offer an ideal blueprint for sustainable battery technology. However, intrinsic instability owing to hydrogen evolution and dendrite formation during the plating process severely compromise the stability of the Zn anode and drastically limit cycling performance. Extending the battery's lifetime at such a complex interface requires a comprehensive approach promotes the formation of a stable and robust solid electrolyte interphase (SEI) layer. Here, we introduce zinc oligoether carboxylates as tuneable dual-function electrolyte additives. The carboxylate group acts as a proton donor, inducing the decomposition of sulfate salt anions to form a ZnS-based SEI, while the oligoether moiety mitigates water activity at the electrode interface, as deduced from the combination of spectroscopic techniques with scanning electrochemical microscopy. By varying the chain length, we find that the longest chain, Zinc (2-[2-[2-(2-methoxyethoxy)ethoxy]ethoxy]acetate)₂, enables long-term cycling under harsher conditions than previously reported, extending cycle life fivefold, sustaining 1000 hours at low current density and high capacity with excellent CE%. This enhancement translates into 98 mAh Zn-MnO2 full pouch cells, supporting the scalability of commercial Zn-based devices by delivering a promising cycle life at low C-rates and high cumulative charge capacity. We hope this discovery will speed up the development of commercial Zn-MnO2 aqueous batteries. Physical sciences/Materials science/Materials for energy and catalysis/Batteries Physical sciences/Chemistry/Electrochemistry/Batteries Full Text Additional Declarations There is NO Competing Interest. Supplementary Files BrownetalSINatComm.pdf Zinc-oligoether carboxylate salts as electrolyte additives for aqueous Zn metal batteries Cite Share Download PDF Status: Published Journal Publication published 20 Dec, 2025 Read the published version in Nature Communications → 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. 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