CAS OpenIR  > 湿法冶金清洁生产技术国家工程实验室
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
Source PublicationACS CATALYSIS
ISSN2155-5435
Volume7Issue:9Pages:6198-6206
Abstract

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.

KeywordC3n4 Photocatalysis Ozone In Situ Epr Dmpo Reactive Oxygen Species
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences
DOI10.1021/acscatal.7b02180
Indexed BySCI
Language英语
WOS KeywordGRAPHITIC CARBON NITRIDE ; SOLAR PHOTOCATALYTIC OZONATION ; WASTE-WATER ; EMERGING CONTAMINANTS ; HYDROGEN-PEROXIDE ; CHARGE-TRANSFER ; SPIN-RESONANCE ; OXALIC-ACID ; G-C3N4 ; OXIDATION
WOS Research AreaChemistry
WOS SubjectChemistry, Physical
Funding OrganizationNational 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 IDWOS:000410005700073
Citation statistics
Cited Times:38[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.ipe.ac.cn/handle/122111/23237
Collection湿法冶金清洁生产技术国家工程实验室
Affiliation1.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
Recommended Citation
GB/T 7714
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.
Files in This Item:
File Name/Size DocType Version Access License
Fast Electron Transf(1839KB)期刊论文出版稿限制开放CC BY-NC-SAApplication Full Text
Related Services
Recommend this item
Bookmark
Usage statistics
Export to Endnote
Google Scholar
Similar articles in Google Scholar
[Xiao, Jiadong]'s Articles
[Rabeah, Jabor]'s Articles
[Yang, Jin]'s Articles
Baidu academic
Similar articles in Baidu academic
[Xiao, Jiadong]'s Articles
[Rabeah, Jabor]'s Articles
[Yang, Jin]'s Articles
Bing Scholar
Similar articles in Bing Scholar
[Xiao, Jiadong]'s Articles
[Rabeah, Jabor]'s Articles
[Yang, Jin]'s Articles
Terms of Use
No data!
Social Bookmark/Share
All comments (0)
No comment.
 

Items in the repository are protected by copyright, with all rights reserved, unless otherwise indicated.