PMID- 37421725 OWN - NLM STAT- MEDLINE DCOM- 20230925 LR - 20230925 IS - 1095-8630 (Electronic) IS - 0301-4797 (Linking) VI - 345 DP - 2023 Nov 1 TI - Zero-valent iron-peroxydisulfate as synergistic co-milling agents for enhanced mechanochemical destruction of 2,4-dichlorophenol: Coupling reduction with oxidation. PG - 118571 LID - S0301-4797(23)01359-2 [pii] LID - 10.1016/j.jenvman.2023.118571 [doi] AB - Mechanochemical (MC) remediation with zero-valent iron (ZVI) as co-milling agent enables the non-combustion and solvent-free disposal of solid halogenated organic pollutants (HOPs) via solid-phase reaction, but suffers from incomplete dechlorination (especially for less chlorinated chemicals). Herein, a reduction-oxidation coupling strategy using ZVI and peroxydisulfate as synergistic (ZVI-PDS) co-milling agents was investigated, with 2,4-dichlorophenol (2,4-DCP) as probe contaminant. By revisiting the MC destruction process of 2,4-DCP by ZVI, the contribution of both reductive and oxidative routes is confirmed, and the inefficient *OH generation is addressed. With ball-to-material and reagent-to-pollutant mass ratios of 30:1 and 13:1, respectively, ZVI-PDS achieves higher dechlorination ratio (86.8%) for 2,4-DCP within 5 h, outcompeting sole ZVI (40.3%) or PDS (33.9%), due to the accumulation of numerous SO(4)(*-). As suggested by a two-compartment kinetic model, the optimal ZVI/PDS molar ratio of 4:1 is determined, which balances the relative contribution of reductive/oxidative routes and leads to a maximum mineralization efficiency of 77.4%. The analysis on product distribution verifies the generation of dechlorinated, ring-opening and minor coupling products (with low acute toxicity). This work validates the necessity to couple reduction with oxidation in MC destruction for solid HOPs, and may provide information on reagent formulation. CI - Copyright (c) 2023 Elsevier Ltd. All rights reserved. FAU - Song, Ludi AU - Song L AD - Collaborative Innovation Center of Yangtze River Delta Region Green Pharmaceuticals, Zhejiang University of Technology, Hangzhou, 310014, China; College of Environment, Zhejiang University of Technology, Hangzhou, 310014, China. FAU - Lin, Lvren AU - Lin L AD - College of Environment, Zhejiang University of Technology, Hangzhou, 310014, China. FAU - Wei, Wenjia AU - Wei W AD - College of Environment, Zhejiang University of Technology, Hangzhou, 310014, China. FAU - Zhang, Shengkun AU - Zhang S AD - Department of Environmental Engineering, Zhejiang University, Hangzhou, 310058, China. FAU - Wan, Lei AU - Wan L AD - Department of Environmental Engineering, Zhejiang University, Hangzhou, 310058, China. FAU - Lou, Zimo AU - Lou Z AD - Collaborative Innovation Center of Yangtze River Delta Region Green Pharmaceuticals, Zhejiang University of Technology, Hangzhou, 310014, China; College of Environment, Zhejiang University of Technology, Hangzhou, 310014, China. Electronic address: louzimo@zjut.edu.cn. FAU - Yu, Jianming AU - Yu J AD - Collaborative Innovation Center of Yangtze River Delta Region Green Pharmaceuticals, Zhejiang University of Technology, Hangzhou, 310014, China; College of Environment, Zhejiang University of Technology, Hangzhou, 310014, China. Electronic address: yjm@zjut.edu.cn. FAU - Xu, Xinhua AU - Xu X AD - Department of Environmental Engineering, Zhejiang University, Hangzhou, 310058, China. Electronic address: xuxinhua@zju.edu.cn. LA - eng PT - Journal Article DEP - 20230706 PL - England TA - J Environ Manage JT - Journal of environmental management JID - 0401664 RN - E1UOL152H7 (Iron) RN - R669TG1950 (2,4-dichlorophenol) RN - 0 (Environmental Pollutants) RN - 0 (Water Pollutants, Chemical) SB - IM MH - Iron/analysis MH - *Environmental Pollutants/analysis MH - Oxidation-Reduction MH - *Water Pollutants, Chemical/analysis OTO - NOTNLM OT - Dechlorination OT - Halogenated organic pollutants OT - Mechanochemistry OT - Peroxydisulfate OT - Zero-valent iron 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- 2023/07/09 01:07 MHDA- 2023/09/25 06:42 CRDT- 2023/07/08 18:02 PHST- 2023/05/14 00:00 [received] PHST- 2023/06/30 00:00 [revised] PHST- 2023/07/02 00:00 [accepted] PHST- 2023/09/25 06:42 [medline] PHST- 2023/07/09 01:07 [pubmed] PHST- 2023/07/08 18:02 [entrez] AID - S0301-4797(23)01359-2 [pii] AID - 10.1016/j.jenvman.2023.118571 [doi] PST - ppublish SO - J Environ Manage. 2023 Nov 1;345:118571. doi: 10.1016/j.jenvman.2023.118571. Epub 2023 Jul 6.