PMID- 37920955 OWN - NLM STAT- MEDLINE DCOM- 20231115 LR - 20231115 IS - 1520-5851 (Electronic) IS - 0013-936X (Linking) VI - 57 IP - 45 DP - 2023 Nov 14 TI - Water Flow-Driven Coupling Process of Anodic Oxygen Evolution and Cathodic Oxygen Activation for Water Decontamination and Prevention of Chlorinated Byproducts. PG - 17404-17414 LID - 10.1021/acs.est.3c02256 [doi] AB - Electrochemical advanced oxidation process (EAOP) is a promising technology for decentralized water decontamination but is subject to parasitic anodic oxygen evolution and formation of toxic chlorinated byproducts in the presence of Cl(-). To address this issue, we developed a novel electrolytic process by water flow-driven coupling of anodic oxygen evolution reaction (OER) and cathodic molecular oxygen activation (MOA). When water flows from anode to cathode, O(2) produced from OER is carried by water through convection, followed by being activated by atomic hydrogen (H*) on Pd cathode to produce (*)OH. The water flow-driven OER/MOA process enables the anode to be polarized at low potential (1.7 V vs SHE) that is lower than that of conventional EAOP whose (*)OH is produced from direct water oxidation (>2.3 V vs SHE). At a flow rate of 30 mL min(-1), the process could achieve 94.8% removal of 2,4-dichlorophenol (2,4-DCP) and 71.5% removal of chemical oxygen demand (COD) within 45 min at an anode potential of 1.7 V vs SHE and cathode potential of -0.5 V vs SHE. To achieve the comparable 2,4-DCP removal performance, 4.3-fold higher energy consumption was needed for the conventional EAOP with titanium suboxide anode (anode potential of 2.9 V vs SHE), but current efficiency declined by 3.5 folds. Unlike conventional EAOP, chlorate and perchlorate were not detected in the OER/MOA process, because low anode potential <2.0 V vs SHE was thermodynamically unfavorable for the formation of chlorinated byproducts by anodic oxidation, indicated by theoretical calculations and experimental data. This study provides a proof-in-concept demonstration of water flow-driven OER/MOA process, representing a paradigm shift of electrochemical technology for water decontamination and prevention of chlorinated byproducts, making electrochemical water decontamination more efficient, more economic, and more sustainable. FAU - Wei, Rui AU - Wei R AD - State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China. FAU - Pei, Shuzhao AU - Pei S AUID- ORCID: 0000-0001-5813-6857 AD - State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China. FAU - Yu, Yuan AU - Yu Y AD - State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China. FAU - Zhang, Jinna AU - Zhang J AD - State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China. FAU - Liu, Yanbiao AU - Liu Y AUID- ORCID: 0000-0001-8404-3806 AD - College of Environmental Science and Engineering, Textile Pollution Controlling Engineering Center of the Ministry of Ecology and Environment, Donghua University, Shanghai 201620, China. FAU - You, Shijie AU - You S AUID- ORCID: 0000-0001-8178-9418 AD - State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China. LA - eng PT - Journal Article PT - Research Support, Non-U.S. Gov't DEP - 20231103 PL - United States TA - Environ Sci Technol JT - Environmental science & technology JID - 0213155 RN - 059QF0KO0R (Water) RN - S88TT14065 (Oxygen) RN - 0 (Water Pollutants, Chemical) SB - IM MH - *Water MH - Oxygen MH - Decontamination MH - Electrolysis MH - Oxidation-Reduction MH - Electrodes MH - *Water Pollutants, Chemical/chemistry OTO - NOTNLM OT - chlorinated byproducts OT - electrochemical advanced oxidation process OT - molecular oxygen activation OT - oxygen evolution reaction OT - water flow-driven EDAT- 2023/11/03 06:44 MHDA- 2023/11/15 06:43 CRDT- 2023/11/03 04:32 PHST- 2023/11/15 06:43 [medline] PHST- 2023/11/03 06:44 [pubmed] PHST- 2023/11/03 04:32 [entrez] AID - 10.1021/acs.est.3c02256 [doi] PST - ppublish SO - Environ Sci Technol. 2023 Nov 14;57(45):17404-17414. doi: 10.1021/acs.est.3c02256. Epub 2023 Nov 3.