PMID- 36804632 OWN - NLM STAT- MEDLINE DCOM- 20230313 LR - 20230313 IS - 1879-1298 (Electronic) IS - 0045-6535 (Linking) VI - 322 DP - 2023 May TI - Effective degradation of 2,4,4'-trichlorodiphenyl by Fe(3)C@Fe-800 activated peroxymonosulfate: Superoxide radical and singlet oxygen-dominated advanced oxidation process. PG - 138164 LID - S0045-6535(23)00431-9 [pii] LID - 10.1016/j.chemosphere.2023.138164 [doi] AB - Polychlorinated biphenyls (PCBs) degradation by peroxymonosulfate (PMS) activation through *OH and SO(4)(*-) radical oxidation process was the effective technology in the last decades; however, there were few research focusing on removing PCBs by O(2)(*-) and (1)O(2) induced by PMS activation. In this work, 90.86% of 2,4,4-trichlorodiphenyl (PCB 28) was degraded by 0.3 g/L Fe(3)C@Fe-800 activated 0.5 mM PMS system under the synergistic action of O(2)(*-) and (1)O(2). The structures of Fe(3)C@Fe-800 were identified by Scanning electron microscope (SEM), High resolution-transmission electron microscopy (HR-TEM), X-ray photoelectron spectroscopy (XPS), Brunauer-Emmett-Teller (BET), Raman spectra and Fourier transform infrared (FT-IR) spectra. Electron paramagnetic resonance (EPR) measurements and quenching tests verified that O(2)(*-) and (1)O(2) were the primary reactive species in Fe(3)C@Fe-800/PMS/PCB 28 ternary reaction system. Density functional theory (DFT), Linear sweep voltammetry (LSV), and chronoamperometry test revealed that electron-deficient Fe atoms on Fe(3)C were the main active sites in Fe(3)C@Fe-800 for PMS activation to generate (1)O(2). Unlike the reported *OH and SO(4)(*-) mediated degradation induced by the iron-based catalyst, both O(2)(*-) and (1)O(2) contributed to PCB 28 degradation: nucleophilic dichlorination reaction by O(2)(*-) and then ring-open oxidation process by (1)O(2). Fe(3)C@Fe-800/PMS system had excellent catalytic performance under different reaction conditions and possessed desirable inorganic salt and natural organic matter resistance. This work elucidated the important role of Fe(3)C in PMS activation to generate O(2)(*-) and (1)O(2) for PCB 28 decontamination by nonradical way and provided a clue to design rationally catalysts in polychlorinated biphenyl pollution remediation. CI - Copyright (c) 2023 Elsevier Ltd. All rights reserved. FAU - Li, Jie AU - Li J AD - School of Environment and Energy, South China University of Technology, Guangzhou, 510006, China. FAU - Yin, Hua AU - Yin H AD - School of Environment and Energy, South China University of Technology, Guangzhou, 510006, China; Key Laboratory of Ministry of Education on Pollution Control and Ecosystem Restoration in Industry Clusters, Guangzhou, 510006, China; Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling, Guangzhou, 510006, China. Electronic address: huayin@scut.edu.cn. FAU - Luo, Haoyu AU - Luo H AD - School of Environment and Energy, South China University of Technology, Guangzhou, 510006, China. FAU - Li, Yingchao AU - Li Y AD - School of Environment and Energy, South China University of Technology, Guangzhou, 510006, China. FAU - Rong, Xufa AU - Rong X AD - School of Environment and Energy, South China University of Technology, Guangzhou, 510006, China. FAU - Dang, Zhi AU - Dang Z AD - School of Environment and Energy, South China University of Technology, Guangzhou, 510006, China; Key Laboratory of Ministry of Education on Pollution Control and Ecosystem Restoration in Industry Clusters, Guangzhou, 510006, China; Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling, Guangzhou, 510006, China. LA - eng PT - Journal Article DEP - 20230217 PL - England TA - Chemosphere JT - Chemosphere JID - 0320657 RN - 22047-43-4 (peroxymonosulfate) RN - 11062-77-4 (Superoxides) RN - 844ODP31Q0 (2,4,4'-trichlorobiphenyl) RN - DFC2HB4I0K (Polychlorinated Biphenyls) RN - 17778-80-2 (Singlet Oxygen) RN - 0 (Peroxides) SB - IM MH - *Superoxides MH - *Polychlorinated Biphenyls MH - Singlet Oxygen MH - Spectroscopy, Fourier Transform Infrared MH - Peroxides/chemistry OTO - NOTNLM OT - 2,4',4-trichlorodiphenyl OT - Degradation OT - Fe(3)C OT - Nonradical pathway OT - PMS COIS- Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper. EDAT- 2023/02/23 06:00 MHDA- 2023/03/14 06:00 CRDT- 2023/02/22 08:53 PHST- 2022/11/24 00:00 [received] PHST- 2023/01/26 00:00 [revised] PHST- 2023/02/14 00:00 [accepted] PHST- 2023/02/23 06:00 [pubmed] PHST- 2023/03/14 06:00 [medline] PHST- 2023/02/22 08:53 [entrez] AID - S0045-6535(23)00431-9 [pii] AID - 10.1016/j.chemosphere.2023.138164 [doi] PST - ppublish SO - Chemosphere. 2023 May;322:138164. doi: 10.1016/j.chemosphere.2023.138164. Epub 2023 Feb 17.