Developing Co-Ni Dual-Atom Catalysts with Synergistic Redox Capacity Via Coordination Self-Assembly and Nano-Confinement Effect

Developing Co-Ni Dual-Atom Catalysts with Synergistic Redox Capacity Via Coordination Self-Assembly and Nano-Confinement Effect | 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 Developing Co-Ni Dual-Atom Catalysts with Synergistic Redox Capacity Via Coordination Self-Assembly and Nano-Confinement Effect xing liu, Yuchen Su, Mengna Feng, Ke Wang, Qinghai Ma, Yudong Li, and 1 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-6521564/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 Combining CO2 reduction and toluene oxidation through photocatalysis is crucial for achieving carbon neutrality and producing high-value chemical products. Herein, a unique Co/Ni diatom-loaded ultrathin carbon nitride (CoSA-NiSA/UCN) has been meticulously synthesized using an innovative strategy of coordination self-assembly and nano-confinement effect. Molecular dynamics simulations (MD) and CO2 temperature-programmed desorption (CO2-TPD) techniques were employed to investigate CO2 with enhanced diffusion and mass transfer capabilities in real-world environments. Experimental and theoretical characterizations show that Co/Ni single atoms act as electron co-catalysts and hole co-catalysts, to effectively modulate the microenvironment on the two-dimensional CN surface and maintain the strongest redox capacity at the position of the conduction/valence band while achieving the effective separation of electron and hole pairs. When toluene was utilized as the sacrificial agent and reactant, the CoSA-NiSA/UCN photocatalytic reduction of CO2 to CO rate of 225.8 μmol g-1 h-1, and the oxidation of toluene to benzaldehyde rate of 486.9 μmol g-1 h-1 (selectivity 82.6%). Femtosecond transient absorption spectroscopy (fs-TA), Kelvin probe force microscopy (KPFM), and theoretical calculations reveal that the simultaneous presence of Co/Ni dual-atom reduces the free energy of *COOH production and enhances the ultrafast kinetic processes of proton coupling and electron-hole transfer. This study introduces a new approach to single-atom synthesis and logically advances the exploration of photogenerated carriers' potential in photocatalysts. Physical sciences/Energy science and technology/Carbon capture and storage Earth and environmental sciences/Environmental sciences/Environmental chemistry/Environmental monitoring Full Text Additional Declarations There is NO Competing Interest. Supplementary Files SupporttingInfo.docx Supportting Info 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-6521564","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":451843611,"identity":"8eabbea1-3394-49d7-802e-6a3f1e3cbcbf","order_by":0,"name":"xing 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Herein, a unique Co/Ni diatom-loaded ultrathin carbon nitride (CoSA-NiSA/UCN) has been meticulously synthesized using an innovative strategy of coordination self-assembly and nano-confinement effect. Molecular dynamics simulations (MD) and CO2 temperature-programmed desorption (CO2-TPD) techniques were employed to investigate CO2 with enhanced diffusion and mass transfer capabilities in real-world environments. Experimental and theoretical characterizations show that Co/Ni single atoms act as electron co-catalysts and hole co-catalysts, to effectively modulate the microenvironment on the two-dimensional CN surface and maintain the strongest redox capacity at the position of the conduction/valence band while achieving the effective separation of electron and hole pairs. 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