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Herein, a \u03c0\u2010conjugated covalent organic framework (Cu@PCT\u2010COF) featuring atomically dispersed Cu\u2010N\n                    <jats:sub>2<\/jats:sub>\n                    coordination sites is reported, which synergistically integrates visible\u2010light harvesting and peroxydisulfate (PDS) activation for efficient photocatalytic degradation of 5\u2010fluorouracil (5\u2010FU). The integration of an extended \u03c0\u2010conjugated backbone with atomically dispersed Cu\u2010N\n                    <jats:sub>2<\/jats:sub>\n                    sites forms a dual\u2010channel electron transport pathway, which significantly enhances interfacial charge transfer and expedites reactive oxygen species (ROS) generation. Driven by this dual\u2010channel electron transport pathway, Cu@PCT\u2010COF achieves 100% removal of 5\u2010FU within 15\u00a0min, which is 4.7 times higher than that of the PCT\u2010COF\/PDS\/vis system and over 10 times greater than systems lacking either vis or PDS. Furthermore, the catalyst exhibits excellent stability, recyclability, and performance across varied pH and ionic conditions, and shows broad\u2010spectrum activity toward diverse pollutants. EPR and quenching experiments identify\n                    <jats:sup>\u2022<\/jats:sup>\n                    OH and SO\n                    <jats:sub>4<\/jats:sub>\n                    <jats:sup>\u2022\u2212<\/jats:sup>\n                    as the primary ROS. Moreover, toxicity analysis and HPLC\u2010MS\/MS reveal a defluorination\u2010initiated ring cleavage pathway, effectively reducing ecological risks. This work offers a promising strategy that leverages \u03c0\u2010electron delocalization and single\u2010atom engineering to realize efficient photocatalytic remediation of fluorinated contaminants.\n                  <\/jats:p>","DOI":"10.1002\/smll.202508775","type":"journal-article","created":{"date-parts":[[2025,10,28]],"date-time":"2025-10-28T13:34:04Z","timestamp":1761658444000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Dual\u2010Channel Electron Modulation via Cu\u2010N\n                    <sub>2<\/sub>\n                    Sites and \u03c0\u2010Conjugated Framework in COF for Enhanced Photocatalytic Degradation of Fluorinated Pharmaceuticals"],"prefix":"10.1002","volume":"21","author":[{"given":"Yaohong","family":"Zhong","sequence":"first","affiliation":[{"name":"Research Center for Eco\u2010environmental Engineering School of Environment and Civil Engineering Dongguan University of Technology  Dongguan 523808 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hui","family":"Wang","sequence":"additional","affiliation":[{"name":"Institute of Chemistry Humboldt University of Berlin  12489 Berlin Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hui","family":"Lin","sequence":"additional","affiliation":[{"name":"Research Center for Eco\u2010environmental Engineering School of Environment and Civil Engineering Dongguan University of Technology  Dongguan 523808 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yongkang","family":"Fan","sequence":"additional","affiliation":[{"name":"Research Center for Eco\u2010environmental Engineering School of Environment and Civil Engineering Dongguan University of Technology  Dongguan 523808 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhiqun","family":"Xie","sequence":"additional","affiliation":[{"name":"Centre for Water Technology &amp; 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