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An electro-Fenton (EF) process, utilizing in situ generated hydrogen peroxide (H2O2), offers effective pollutant degradation. While current electrocatalysts often suffer from low H2O2 selectivity, single-atom catalysts (SACs) have demonstrated superior activity and selectivity. However, their application is limited by poor acidic stability, particularly with nitrogen-coordinated site deactivation under strong oxidation conditions. Herein, a nitrogen-free cobalt single-atom catalyst (BP\u2013Co) was synthesized on defect-rich carbon via ball milling-pyrolysis. BP\u2013Co demonstrates 80% Faradaic efficiency and 10.5 mg cm\u20132 h\u20131 H2O2 yield in acidic media. Both experimental and computational results demonstrate that the presence of surface epoxy groups improves interfacial wettability and electronically tailors the Co\u2013C active sites, thus facilitating *OOH desorption and promoting H2O2 generation. In EF applications, BP\u2013Co achieves 100% removal of thiamphenicol (TAP), 77.9% TOC mineralization, continuous Fe2+ regeneration, and low energy consumption (0.093 kWh (g TOC)\u22121). Moreover, the toxicity of degradation byproducts was significantly reduced. The system performs well across various water matrices and effectively degrades multiple organic pollutants. This study presents a cost-effective, stable strategy for nitrogen-free SACs, advancing water treatment technologies.<\/jats:p>","DOI":"10.1021\/acs.est.5c10994","type":"journal-article","created":{"date-parts":[[2025,10,13]],"date-time":"2025-10-13T08:04:49Z","timestamp":1760342689000},"page":"22318-22329","source":"Crossref","is-referenced-by-count":15,"title":["Synergy\nbetween Surface Epoxy Groups and Co\u2013C\nSites in Nitrogen-Free Single-Atom Catalysts for Electro-Fenton Water\nPurification"],"prefix":"10.1021","volume":"59","author":[{"given":"Jingyuan","family":"Luo","sequence":"first","affiliation":[{"name":"North China Electric Power University , , ,","place":["Beijing, China, 102206"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7584-5695","authenticated-orcid":true,"given":"Yuanzheng","family":"Zhang","sequence":"additional","affiliation":[{"name":"North China Electric Power University , , ,","place":["Beijing, China, 102206"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuxin","family":"Zeng","sequence":"additional","affiliation":[{"name":"Beijing Normal University , , ,","place":["Beijing, China, 100875"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haopeng","family":"Feng","sequence":"additional","affiliation":[{"name":"Anhui University , , ,","place":["Hefei, China, 230601"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huihui","family":"Li","sequence":"additional","affiliation":[{"name":"The University of New South Wales , , , ,","place":["Sydney, New South Wales, Australia, 2052"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5181-195X","authenticated-orcid":true,"given":"Lifeng","family":"Yin","sequence":"additional","affiliation":[{"name":"Beijing Normal University , , ,","place":["Beijing, China, 100875"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2592-3103","authenticated-orcid":true,"given":"Junfeng","family":"Niu","sequence":"additional","affiliation":[{"name":"North China Electric Power University , , ,","place":["Beijing, China, 102206"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2025,10,13]]},"reference":[{"key":"2026081812165865400_cit1","doi-asserted-by":"publisher","first-page":"119876","DOI":"10.1016\/j.watres.2023.119876","article-title":"Source Preventing Mechanism\nof Florfenicol Resistance Risk in Water by VUV\/UV\/Sulfite Advanced\nReduction Pretreatment","volume":"235","author":"Dong","year":"2023","journal-title":"Water Res."},{"key":"2026081812165865400_cit2","doi-asserted-by":"publisher","first-page":"19501","DOI":"10.1021\/acs.est.4c06536","article-title":"Customizable\nThree-Dimensional Printed Zerovalent Iron: An Efficient and Reusable\nFenton-like Reagent for Florfenicol Degradation","volume":"58","author":"Li","year":"2024","journal-title":"Environ. 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