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Sustainable remediation of fluorophenols by O2•−/1O2-mediated oxidative polymerization with synchronous defluorination and continuous-flow demonstration

Journal 2026 · IF 6.6 · 发表于 2026 年 9 月 10 日
作者: Chunke Zhao,Yueying Gao,Jiaye Duan,Shiting Li,Bo Zhang,Ke Ma,Longtao Dang,Gen Wang
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摘要

Polymeric removal of various FPs with concurrent defluorination is achieved in a CuO/PMS system. • FPs are efficiently converted into solid PPO-like polymers with minimal PMS consumption. • 1 O 2 and O 2 •− synergistically drive the polymerization and defluorination of FPs. • Continuous-flow operation over 120 h sustains ∼95% 4-FP removal, confirming practical applicability. Fluorophenols (FPs) are persistent organic pollutants of high concern owing to the extreme stability of their C F bonds. Here we report an oxidative polymerization strategy that enables simultaneous pollutant removal and defluorination by transforming FPs into solid polymers. In a CuO-activated peroxymonosulfate (PMS) system, a superoxide radical (O 2 •− ) and singlet oxygen ( 1 O 2 ) co-mediated oxidation process was established. The system achieved near-complete removal of a series of FPs with different fluorine substitution patterns (2-FP, 4-FP, 2,4-DFP, and 2,3,5,6-TeFP) using minimal oxidant consumption. Polymerization efficiencies ranged from ∼26% to ∼72%, accompanied by significant defluorination (up to ∼74%). Mechanistic studies reveal that FPs are converted into solid poly(phenylene oxide)-like polymers via a nucleophilic aromatic substitution route. Beyond batch performance, the system demonstrated excellent practical viability, with ∼95% removal of 4-FP sustained in a continuous-flow reactor and defluorination remaining as high as ∼47% after prolonged operation. The process also maintained high efficiency under hypersaline and complex water matrices. This integrated defluorination-polymerization approach offers a cost-effective, environmentally benign and operationally stable solution for treating FPs-contaminated wastewaters, shifting the paradigm from conventional mineralization toward sustainable resource recovery. Download: Download high-res image (163KB) Download: Download full-size image