Fast Electron Transfer and (OH)-O-center dot Formation: Key Features for High Activity in Visible-Light-Driven Ozonation with C3N4 Catalysts
Xiao, Jiadong1,2,3; Rabeah, Jabor3; Yang, Jin1; Xie, Yongbing1; Cao, Hongbin1; Brueckner, Angelika3
2017-09-01
发表期刊ACS CATALYSIS
ISSN2155-5435
卷号7期号:9页码:6198-6206
摘要

Photocatalytic ozonation of wastewater pollutants by sunlight is a highly attractive technology close to real application. Understanding this process on the atomic scale and under realistic working conditions is challenging but vital for the rational design of catalysts and photocatalytic decontamination systems. Here we study two highly active C3N4 photocatalysts (bulk C3N4 and a nanosheet-structured C3N4) under simultaneous visible-light irradiation and O-3 bubbling in water by in situ EPR spectroscopy coupled with an online spin trapping technique. The photoexcitation of electrons to the conduction band (CB-e(-)), their further trapping by dissolved O-2 and O-3, and the evolution of reactive oxygen species (ROS) have been semiquantitatively visualized. A dual role of O-3 in boosting the CB-e(-) to (OH)-O-center dot conversion is confirmed: (i) an inlet 2.1 mol % O-3/O-2 gas mixture can trap about 2-3 times more CB-e(-) upon aqueous C3N4 suspension than pure O-2 and further produce (OH)-O-center dot by a robust O-center dot(3)--mediated one-electron-reduction pathway (O-3 -> O-center dot(3)- -> HO3 center dot -> (OH)-O-center dot); (ii) O-3 can readily take CB-e(-) back from O-center dot(3) to form O-center dot(3)-, thus blocking the inefficient H2O2-mediated three-electron-reduction route (O-2 -> O-center dot(2)- -> HO2 center dot H2O2 -> (OH)-O-center dot) but further strengthening the O-center dot(3)--mediated pathway. In the presence of 2.1 mol % O-3/O-2, the (OH)-O-center dot yield increases by 17 and 5 times, and consequently, the mineralization rate constant of oxalic acid increases by 84 and 41 times over bulk C3N4 and NS C3N4, respectively. This work presents an attractive opportunity to boost the yield of ROS species ((OH)-O-center dot) for water purification by visible-light-driven photocatalysis and provides a powerful tool to monitor complex photocatalytic reactions under practical conditions.

关键词C3n4 Photocatalysis Ozone In Situ Epr Dmpo Reactive Oxygen Species
文章类型Article
WOS标题词Science & Technology ; Physical Sciences
DOI10.1021/acscatal.7b02180
收录类别SCI
语种英语
关键词[WOS]GRAPHITIC CARBON NITRIDE ; SOLAR PHOTOCATALYTIC OZONATION ; WASTE-WATER ; EMERGING CONTAMINANTS ; HYDROGEN-PEROXIDE ; CHARGE-TRANSFER ; SPIN-RESONANCE ; OXALIC-ACID ; G-C3N4 ; OXIDATION
WOS研究方向Chemistry
WOS类目Chemistry, Physical
项目资助者National Science Fund for Distinguished Young Scholars of China(51425405) ; Natural Science Foundation of Beijing Municipality(8172043) ; Major Science and Technology Program for Water Pollution Control and Treatment(2014ZX07510-001) ; CAS-DAAD(91637735)
WOS记录号WOS:000410005700073
引用统计
文献类型期刊论文
条目标识符http://ir.ipe.ac.cn/handle/122111/23237
专题湿法冶金清洁生产技术国家工程实验室
作者单位1.Chinese Acad Sci, Inst Proc Engn, Div Environm Technol & Engn, Beijing Engn Res Ctr Proc Pollut Control, Beijing 100190, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Univ Rostock, Leibniz Inst Catalysis eV, Albert Einstein Str 29a, D-18059 Rostock, Germany
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Xiao, Jiadong,Rabeah, Jabor,Yang, Jin,et al. Fast Electron Transfer and (OH)-O-center dot Formation: Key Features for High Activity in Visible-Light-Driven Ozonation with C3N4 Catalysts[J]. ACS CATALYSIS,2017,7(9):6198-6206.
APA Xiao, Jiadong,Rabeah, Jabor,Yang, Jin,Xie, Yongbing,Cao, Hongbin,&Brueckner, Angelika.(2017).Fast Electron Transfer and (OH)-O-center dot Formation: Key Features for High Activity in Visible-Light-Driven Ozonation with C3N4 Catalysts.ACS CATALYSIS,7(9),6198-6206.
MLA Xiao, Jiadong,et al."Fast Electron Transfer and (OH)-O-center dot Formation: Key Features for High Activity in Visible-Light-Driven Ozonation with C3N4 Catalysts".ACS CATALYSIS 7.9(2017):6198-6206.
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