Carbon Surface Crowding and Subsurface Traffic Jam as Drivers for Methane Oxidation Activity and Selectivity on Palladium Surfaces

Carbon Surface Crowding and Subsurface Traffic Jam as Drivers for Methane Oxidation Activity and Selectivity on Palladium Surfaces | 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 Carbon Surface Crowding and Subsurface Traffic Jam as Drivers for Methane Oxidation Activity and Selectivity on Palladium Surfaces Jan Knudsen, Ulrike Küst, Rosemary Jones, Julia Prumbs, Alessandro Namar, and 2 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-5705568/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 20 Aug, 2025 Read the published version in Nature Communications → Version 1 posted You are reading this latest preprint version Abstract Separating how surface and subsurface species affect catalytic function is a challenging task in heterogeneous catalysis, particularly when deposition and segregation take place at reaction conditions. Here, we report on an operando approach to establish surface/subsurface/function correlations. Using temperature modulations we oscillate carbon deposition and segregation over a Pd catalyst. Catalytic composition and function are monitored during methane oxidation with time- and depth-resolved spectroscopy coupled with Fourier analysis. Hereby, we show that the surface coverage of carbon drives partial oxidation to CO, while the subsurface carbon controls the overall methane turnover. Also, we show that a carbon traffic jam in the subsurface leads to a shifting selectivity from H 2 to H 2 O formation. Physical sciences/Chemistry/Catalysis/Heterogeneous catalysis Physical sciences/Physics/Condensed-matter physics/Surfaces, interfaces and thin films Full Text Additional Declarations There is NO Competing Interest. Supplementary Files Graphicalabstract.pdf manuscriptSI.pdf Supporting Information for review Cite Share Download PDF Status: Published Journal Publication published 20 Aug, 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. 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-5705568","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":405654398,"identity":"ec63d2a4-e982-4127-af9d-8328611163ef","order_by":0,"name":"Jan 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