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Superoxide radical-mediated photocatalytic oxidation of phenolic compounds over Ag+/TiO2: Influence of electron donating and withdrawing substituents
Xiao, Jiadong1,2; Xie, Yongbing1; Han, Qingzhen3; Cao, Hongbin1,4; Wang, Yujiao5; Nawaz, Faheem1,2; Duan, Feng1,2
2016-03-05
发表期刊JOURNAL OF HAZARDOUS MATERIALS
ISSN0304-3894
卷号304期号:MAR页码:126-133
摘要A comparative study was constructed to correlate the electronic property of the substituents with the degradation rates of phenolic compounds and their oxidation pathways under UV with Ag+/TiO2 suspensions. It was verified that a weak electron withdrawing substituent benefited photocatalytic oxidation the most, while an adverse impact appeared when a substituent was present with stronger electron donating or withdrawing ability. The addition of p-benzoquinone dramatically blocked the degradation, confirming superoxide radicals (O-center dot(2)-) as the dominant photooxidant, rather than hydroxyl radicals, singlet oxygen or positive holes, which was also independent of the substituent. Hammett relationship was established based on pseudo-first-order reaction kinetics, and it revealed two disparate reaction patterns between center dot O-2(-) and phenolic compounds, which was further verified by the quantum chemical computation on the frontier molecular orbitals and Mulliken charge distributions of center dot O-2(-) and phenolic compounds. It was found that electron donating group (EDG) substituted phenols were more likely nucleophilically attacked by center dot O-2(-), while center dot O-2(-) preferred to electrophilically assault electron withdrawing group (EWG) substituted phenols. Exceptionally, electrophilic and nucleophilic attack by center dot O-2(-) could simultaneously occur in p-chlorophenol degradation, consequently leading to its highest rate constant. Possible reactive positions on the phenolic compounds were also detailedly uncovered. (C) 2015 Elsevier B.V. All rights reserved.
关键词Tio2 Photocatalysis Substituent Phenolic Compounds Superoxide Radical Mechanism
文章类型Article
WOS标题词Science & Technology ; Technology ; Life Sciences & Biomedicine
DOI10.1016/j.jhazmat.2015.10.052
收录类别SCI
语种英语
关键词[WOS]VISIBLE-LIGHT IRRADIATION ; TIO2 AQUEOUS SUSPENSIONS ; DOPED TIO2 ; HYDROTHERMAL SYNTHESIS ; TITANIUM-DIOXIDE ; METAL-IONS ; DEGRADATION ; CARBON ; 4-CHLOROPHENOL ; PHOTODEGRADATION
WOS研究方向Engineering ; Environmental Sciences & Ecology
WOS类目Engineering, Environmental ; Engineering, Civil ; Environmental Sciences
项目资助者National Natural Science Foundation of China(21207133) ; National Science Fund for Distinguished Young Scholars(51425405) ; Major Science and Technology Program for Water Pollution Control and Treatment(2013ZX07209-001 ; 2015ZX07202013-002)
WOS记录号WOS:000367699200015
引用统计
文献类型期刊论文
条目标识符http://ir.ipe.ac.cn/handle/122111/20259
专题多相复杂系统国家重点实验室
作者单位1.Chinese Acad Sci, Beijing Engn Res Ctr Proc Pollut Control, Key Lab Green Proc & Engn,Inst Proc Engn, Natl Engn Lab Hydromet Cleaner Prod Technol, Beijing 100190, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Chinese Acad Sci, Inst Proc Engn, State Key Lab Multiphase Complex Syst, Beijing 100190, Peoples R China
4.Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Tianjin 300072, Peoples R China
5.Univ Sci & Technol Beijing, Dept Chem & Biomed Engn, Beijing, Peoples R China
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Xiao, Jiadong,Xie, Yongbing,Han, Qingzhen,et al. Superoxide radical-mediated photocatalytic oxidation of phenolic compounds over Ag+/TiO2: Influence of electron donating and withdrawing substituents[J]. JOURNAL OF HAZARDOUS MATERIALS,2016,304(MAR):126-133.
APA Xiao, Jiadong.,Xie, Yongbing.,Han, Qingzhen.,Cao, Hongbin.,Wang, Yujiao.,...&Duan, Feng.(2016).Superoxide radical-mediated photocatalytic oxidation of phenolic compounds over Ag+/TiO2: Influence of electron donating and withdrawing substituents.JOURNAL OF HAZARDOUS MATERIALS,304(MAR),126-133.
MLA Xiao, Jiadong,et al."Superoxide radical-mediated photocatalytic oxidation of phenolic compounds over Ag+/TiO2: Influence of electron donating and withdrawing substituents".JOURNAL OF HAZARDOUS MATERIALS 304.MAR(2016):126-133.
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