Reactive Oxygen Pool over Ceria Enables Catalytic Oscillation

Reactive Oxygen Pool over Ceria Enables Catalytic Oscillation | 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 Research Article Reactive Oxygen Pool over Ceria Enables Catalytic Oscillation Jie Yan, Maolin Wang, Junzhong Xie, Yapeng Zhao, Xianghui Shi, and 15 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-9275333/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 Heterogeneous catalytic reactions often exhibit kinetic oscillations—spontaneous, non-equilibrium phenomena occurring across various reaction systems. Despite decades of investigations, the mechanisms that initiate and sustain these oscillations remain elusive. Here we report the discovery of unexpected kinetic oscillations over Pt/CeO 2 catalysts during the competitive oxidation of hydrogen and carbon monoxide at approximately 60°C. Through operando characterization and first-principles mathematical analysis, we uncover the underlying mechanism and existence conditions of oscillations, demonstrating that these oscillations are governed by periodic cycles of ceria reduction and oxidation, gated by CO coverage on Pt. This represents the first demonstration that the reactive oxygen pool of the support can actively induce and sustain catalytic oscillations. These findings redefine metal-support synergy and provide a theoretical formalism for understanding complex non-equilibrium phenomena in heterogeneous catalysis. Catalysis Surface chemistry Full Text Additional Declarations The authors declare no competing interests. Supplementary Files SupplementalMaterial.docx Supplementary Material movieS1.mp4 Movie S1 movieS22.mp4 Movie S2 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-9275333","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":615034278,"identity":"284d747e-af37-4eb9-b6b6-72875bc88715","order_by":0,"name":"Jie Yan","email":"","orcid":"","institution":"College of Chemistry and Molecular Engineering, Peking University","correspondingAuthor":false,"prefix":"","firstName":"Jie","middleName":"","lastName":"Yan","suffix":""},{"id":615034280,"identity":"c0ffd932-b60c-4eeb-8257-b21e09f67800","order_by":1,"name":"Maolin Wang","email":"","orcid":"","institution":"College of Chemistry and Molecular 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Despite decades of investigations, the mechanisms that initiate and sustain these oscillations remain elusive. Here we report the discovery of unexpected kinetic oscillations over Pt/CeO\u003csub\u003e2\u003c/sub\u003e catalysts during the competitive oxidation of hydrogen and carbon monoxide at approximately 60\u0026deg;C. Through \u003cem\u003eoperando\u003c/em\u003e characterization and first-principles mathematical analysis, we uncover the underlying mechanism and existence conditions of oscillations, demonstrating that these oscillations are governed by periodic cycles of ceria reduction and oxidation, gated by CO coverage on Pt. This represents the first demonstration that the reactive oxygen pool of the support can actively induce and sustain catalytic oscillations. 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