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Bicarbonate-enhanced generation of hydroxyl radical by visible light-induced photocatalysis of H2O2 over WO3: Alteration of electron transfer mechanism

Authors
Choi, JaeminKim, Hak-HyeonLee, Ki-MyeongChen, NaKim, Min SikSeo, JiwonLee, DonghyunCho, HaeinKim, Hyoung-ilLee, JaesangLee, HongshinLee, Changha
Issue Date
15-3월-2022
Publisher
ELSEVIER SCIENCE SA
Keywords
Tungsten oxide; Photocatalysis; Hydroxyl radical; Hydrogen peroxide; Bicarbonate
Citation
CHEMICAL ENGINEERING JOURNAL, v.432
Indexed
SCIE
SCOPUS
Journal Title
CHEMICAL ENGINEERING JOURNAL
Volume
432
URI
https://scholar.korea.ac.kr/handle/2021.sw.korea/143122
DOI
10.1016/j.cej.2021.134401
ISSN
1385-8947
Abstract
The generation of hydroxyl radical ((OH)-O-center dot) by visible light-illuminated tungsten oxide (WO3) was found to be significantly improved in the presence of hydrogen peroxide (H2O2) and bicarbonate ion (HCO3-). A ternary system of h nu/WO3/H2O2/HCO3- showed synergistic enhancement in oxidation of benzoic acid (BA, a (OH)-O-center dot probe compound) into hydroxybenzoic acids (HBAs), exhibiting even less consumption of H2O2 than h nu/WO3/H2O2. Analyses of HBAs from BA oxidation (three HBA isomers and O-18-labelled HBA from (H2O2)-O-18) suggested that h nu/WO3/H2O2/HCO3-, contrary to h nu/WO3/H2O2, generated (OH)-O-center dot mainly via one-electron transfer from the conduction band of WO3 to H2O2. The dominant one-electron reduction of H2O2 over HCO3--treated WO3 was further evidenced by Koutecky-Levich plots obtained with a rotating disk electrode setup. Based on different experiments using electron paramagnetic resonance spectroscopy, radical scavengers and probes, (photo-)electrochemical measurements, and density functional theory calculations, the mechanisms underlying the enhanced generation of (OH)-O-center dot by h nu/WO3/H2O2/HCO3- were discussed.
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공과대학 (건축사회환경공학부)
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