RESEARCH PAPER · Communications Chemistry · 2025

Solar-driven defluorination via hydroxyl radical spillover for complete mineralization of organofluorine pollutants without fluoride byproducts

Lei Zheng, Jinglan Zhang, Zhixin Zheng, Chujie Huang, Yilin Xie, Xu‐Bing Li, Fentahun Wondu Dagnaw, Tieyu Wang, Qing‐Xiao Tong, Jing‐Xin Jian

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Abstract

Abstract The recalcitrance of fluorinated organic pollutants—featuring robust Csp²-F and Csp³-F bonds—poses critical challenges to aquatic ecosystems due to their extreme persistence and bioaccumulation. Whereas current destruction strategies suffer from high energy consumption and non-selective, here we present a solar-powered mineralization strategy utilizing cerium oxide/mesoporous silica (CeO2/mSiO2) heterojunction photocatalysts for complete defluorination of organofluorine contaminants, including fluorinated e-waste, fluoro-antibiotics and perfluorinated surfactant. Under visible light irradiation, the optimized 5%CeO2/mSiO2 achieved 91.1 ± 3.2% octafluorobiphenyl (OFB) and 97.7 ± 2.8% fleroxacin (FLE) degradations within 6 h. Notably, the ‘forever chemical’ perfluorooctanesulfonic acid (PFOS) can be effectively destructed, achieving a maximum of 25.9 ± 2.7% reduction in 5 days under sunshine, outperforming parallel experiments conducted without a catalyst (~0%). This process notably avoids the evolution of fluoride ions. Theoretical calculations reveal that the removal of C-F bonds by photogenerated hydroxyl radical is thermodynamically superior to hydroxyl-mediated defluorination. This work establishes an energy-efficient paradigm for eradicating “forever chemicals” without secondary pollution, advancing sustainable water remediation technologies.

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