High Throughput Exsolution Design of CO2 Reduction Reaction Interface in a Copper/High-Entropy Oxide Tandem Electrode

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Abstract The entropy design paradigm is yielding advanced materials for many societally crucial applications. While most work focuses on single-phase materials, there are vast opportunities to integrate entropy-designed materials into novel composites. Here we develop a nanocomposite design strategy using exsolution-self-assembly to fabricate Cu nanorods in an entropy-stabilized oxide. Atomic-scale electron probes and energetic calculations elucidate how exsolution-self-assembly is tunable using knowledge of point defect interactions. We leverage this to then demonstrate a high-throughput synthesis and screening strategy to fabricate a library of Cu-ESO tandem CO2 reduction reaction (CO2RR) electrodes. Electrocatalytic mapping and localized physicochemical analyses reveal structure-property relationships between local Cu valence and CO2RR activity, identifying operating potentials and electrode surface chemistries that favor CO2RR over competitive hydrogen evolution. This high-throughput synthesis-screening approach can accelerate development of advanced electrocatalysts and nanocomposite materials for many applications given its compatibility with entropy-designed materials and physical vapor deposition at/near silicon volume manufacturing temperatures.
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High Throughput Exsolution Design of CO2 Reduction Reaction Interface in a Copper/High-Entropy Oxide Tandem Electrode | 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 High Throughput Exsolution Design of CO2 Reduction Reaction Interface in a Copper/High-Entropy Oxide Tandem Electrode William Bowman, ShengQuan Xuan, Tamilselvi Gurusamy, Xin Wang, and 8 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-4481093/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 The entropy design paradigm is yielding advanced materials for many societally crucial applications. While most work focuses on single-phase materials, there are vast opportunities to integrate entropy-designed materials into novel composites. Here we develop a nanocomposite design strategy using exsolution-self-assembly to fabricate Cu nanorods in an entropy-stabilized oxide. Atomic-scale electron probes and energetic calculations elucidate how exsolution-self-assembly is tunable using knowledge of point defect interactions. We leverage this to then demonstrate a high-throughput synthesis and screening strategy to fabricate a library of Cu-ESO tandem CO2 reduction reaction (CO2RR) electrodes. Electrocatalytic mapping and localized physicochemical analyses reveal structure-property relationships between local Cu valence and CO2RR activity, identifying operating potentials and electrode surface chemistries that favor CO2RR over competitive hydrogen evolution. This high-throughput synthesis-screening approach can accelerate development of advanced electrocatalysts and nanocomposite materials for many applications given its compatibility with entropy-designed materials and physical vapor deposition at/near silicon volume manufacturing temperatures. Physical sciences/Materials science/Materials for energy and catalysis/Electrocatalysis Physical sciences/Materials science/Nanoscale materials/Synthesis and processing Electrocatalyst CO2 reduction reaction entropy stabilized oxide exsolution self-assembly thin film scanning electrochemical cell microscopy Full Text Additional Declarations There is NO Competing Interest. Supplementary Files HEOCuv12SI240526.pdf Supplementary Information 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. 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