Modulating Coordinate Site Occupancy in High-entropy Spinel Electrocatalysts

Modulating Coordinate Site Occupancy in High-entropy Spinel Electrocatalysts | 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 Modulating Coordinate Site Occupancy in High-entropy Spinel Electrocatalysts Xiaolin Zheng, Jihyun Baek, Yuzhe Li, Kiran Hamkins, Angel Garcia-Esparza, and 11 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7687221/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 20 Mar, 2026 Read the published version in Nature Communications → Version 1 posted You are reading this latest preprint version Abstract High-entropy spinel oxides (HESOs) allow for tunable electronic structures and improved electrocatalytic properties through multi-cation engineering, yet understanding and controlling site-specific cation distributions remains a key challenge. Here, we modulate cationic coordination site occupancy between tetrahedral and octahedral sites in a Co–Fe–Cr–Mn–Ni framework by adding a sixth cation with a different site preference energy (e.g., Zn, Ga, Mg, or Al). Zn preferentially occupies tetrahedral sites, which increases octahedral occupancy of Co. Such site modification is confirmed by density functional theory, synchrotron X-ray absorption spectroscopy, and magnetic circular dichroism. Particularly, Zn-HESO shows the highest occupancy of Co3+ and Co2+ in octahedral sites, leading to more active sites for oxygen evolution reaction, increased electrical conductivity, and greater catalytic activity and stability among different HESOs. Adding a selected cation effectively tunes coordination site occupation in spinels, showing a clear structure-property relationship and providing a clue for the development of next-generation multicomponent catalysts. Physical sciences/Materials science/Materials for energy and catalysis/Electrocatalysis Physical sciences/Chemistry/Electrochemistry/Electrocatalysis Full Text Additional Declarations There is NO Competing Interest. Supplementary Files SIModulatingCoordinateSiteOccupancyinHighentropySpinelElectrocatalysts.docx Supplementary Information Cite Share Download PDF Status: Published Journal Publication published 20 Mar, 2026 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. 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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-7687221","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":526695441,"identity":"72052f9b-9b4d-4518-ad37-4454fd6524c6","order_by":0,"name":"Xiaolin 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