Coordination engineering enables highly selective generation of carbonate radical for enhanced Fenton-like reactions

Coordination engineering enables highly selective generation of carbonate radical for enhanced Fenton-like reactions | 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 Coordination engineering enables highly selective generation of carbonate radical for enhanced Fenton-like reactions Xianjun Tan This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7847817/v1 This work is licensed under a CC BY 4.0 License Status: Posted Version 1 posted You are reading this latest preprint version Graphical Abstract Abstract Overturning the conventional wisdom, recent studies demonstrated that bicarbonate ions (HCO) serve as promoters instead of inhibitors in heterogeneous Fenton-like processes. Nevertheless, the interfacial activation mechanisms of HCO and HO remain insufficiently understood, hindering the rational development of efficient catalytic processes. Herein, we report a coordination-regulated Co single-atom catalyst (SAC) that enables a highly selective pathway for carbonate radical (CO) generation. By constructing a six-coordinated CoN configuration (Co-N/C-T), the system achieved rapid and efficient degradation of sulfamethoxazole (SMX, 96.9%) within 60 min, with CO accounting for 98.9% of the total reactivity. Mechanistic insights from Fourier-transform infrared (FTIR) and density functional theory (DFT) calculations revealed the preferential adsorption and dissociation of peroxymonocarbonate (HCO) intermediate at CoN sites, facilitating selective generation of CO as the dominant reactive oxygen species (ROS). The Co-N/C-T Fenton-like system also exhibited robust performance and excellent recyclability at environmentally relevant concentrations across various realistic water matrices. Furthermore, a structure-reactivity correlation grounded in electronic descriptors revealed the system’s high selectivity toward electron-rich amine-containing antibiotics and their analogues, offering a targeted strategy for contaminant removal under complex water matrices. These findings provide mechanistic insights for advancing next-generation Fenton-like systems across diverse water treatment scenarios. Earth and environmental sciences/Environmental sciences/Environmental chemistry/Pollution remediation Physical sciences/Chemistry/Catalysis/Heterogeneous catalysis Full Text Additional Declarations There is NO Competing Interest. Supplementary Files SupportingInformation.docx Supporting Information GA.png Graphical abstract 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-7847817","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":530244966,"identity":"0a3bd953-bffc-43a7-a731-79b7695b3d0b","order_by":0,"name":"Xianjun 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