Water Flow-Driven Coupling Process of Anodic Oxygen Evolution and Cathodic Oxygen Activation for Water Decontamination and Prevention of Chlorinated Byproducts

Rui Wei; Shuzhao Pei; Yuan Yu; Jinna Zhang; Yanbiao Liu; Shijie You

doi:10.1021/acs.est.3c02256

Water Flow-Driven Coupling Process of Anodic Oxygen Evolution and Cathodic Oxygen Activation for Water Decontamination and Prevention of Chlorinated Byproducts

Rui Wei
, Shuzhao Pei
, Yuan Yu
, Jinna Zhang
, Yanbiao Liu
, Shijie You^*

^*Corresponding author for this work

School of Environment, Harbin Institute of Technology
Donghua University

Research output: Contribution to journal › Article › peer-review

35 Scopus citations

Abstract

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, O₂ 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.

Original language	English
Pages (from-to)	17404-17414
Number of pages	11
Journal	Environmental Science and Technology
Volume	57
Issue number	45
DOIs	https://doi.org/10.1021/acs.est.3c02256
State	Published - 14 Nov 2023
Externally published	Yes

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

Keywords

chlorinated byproducts
electrochemical advanced oxidation process
molecular oxygen activation
oxygen evolution reaction
water flow-driven

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10.1021/acs.est.3c02256

Cite this

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title = "Water Flow-Driven Coupling Process of Anodic Oxygen Evolution and Cathodic Oxygen Activation for Water Decontamination and Prevention of Chlorinated Byproducts",

abstract = "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, O2 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.",

keywords = "chlorinated byproducts, electrochemical advanced oxidation process, molecular oxygen activation, oxygen evolution reaction, water flow-driven",

author = "Rui Wei and Shuzhao Pei and Yuan Yu and Jinna Zhang and Yanbiao Liu and Shijie You",

note = "Publisher Copyright: {\textcopyright} 2023 American Chemical Society",

year = "2023",

month = nov,

day = "14",

doi = "10.1021/acs.est.3c02256",

language = "英语",

volume = "57",

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publisher = "American Chemical Society",

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}

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T1 - Water Flow-Driven Coupling Process of Anodic Oxygen Evolution and Cathodic Oxygen Activation for Water Decontamination and Prevention of Chlorinated Byproducts

AU - Wei, Rui

AU - Pei, Shuzhao

AU - Yu, Yuan

AU - Zhang, Jinna

AU - Liu, Yanbiao

AU - You, Shijie

PY - 2023/11/14

Y1 - 2023/11/14

N2 - 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, O2 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.

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, O2 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.

KW - chlorinated byproducts

KW - electrochemical advanced oxidation process

KW - molecular oxygen activation

KW - oxygen evolution reaction

KW - water flow-driven

UR - https://www.scopus.com/pages/publications/85176968629

U2 - 10.1021/acs.est.3c02256

DO - 10.1021/acs.est.3c02256

M3 - 文章

C2 - 37920955

AN - SCOPUS:85176968629

SN - 0013-936X

VL - 57

SP - 17404

EP - 17414

JO - Environmental Science and Technology

JF - Environmental Science and Technology

IS - 45

ER -

Water Flow-Driven Coupling Process of Anodic Oxygen Evolution and Cathodic Oxygen Activation for Water Decontamination and Prevention of Chlorinated Byproducts

Abstract

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Keywords

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