Insight into (OH)-O-center dot and O-2(center dot-) formation in heterogeneous catalytic ozonation by delocalized electrons and surface oxygen-containing functional groups in layered-structure nanocarbons 机翻标题: 暂无翻译,请尝试点击翻译按钮。

来源
Chemical engineering journal
年/卷/期
2019 / 357 /
页码
655-666
ISSN号
1385-8947
作者单位
Chengdu Univ Technol, State Key Lab Geohazard Prevent & Geoenvironm Pro, Chengdu, Sichuan, Peoples R China;Beijing Forestry Univ, Coll Environm Sci & Engn, Beijing Key Lab Source Control Technol Water Poll, Beijing 100083, Peoples R China;Chinese Res Inst Environm Sci, State Key Lab Environm Criteria & Risk Assessment, Beijing 100012, Peoples R China;Beijing Forestry Univ, Coll Environm Sci & Engn, Beijing Key Lab Source Control Technol Water Poll, Beijing 100083, Peoples R China;Beijing Forestry Univ, Coll Environm Sci & Engn, Beijing Key Lab Source Control Technol Water Poll, Beijing 100083, Peoples R China;Beijing Univ Civil Engn & Architecture, Key Lab Urban Storm Water Syst & Water Environm, Minist Educ, Beijing 100044, Peoples R China;Beijing Forestry Univ, Coll Environm Sci & Engn, Beijing Key Lab Source Control Technol Water Poll, Beijing 100083, Peoples R China;
作者
Pu, Shengyan;Song, Zilong;Xu, Bingbing;Qi, Fei;Zhang, Yuting;Yuan, Donghai;Liu, Chao;
摘要
Owing to their unique structure and specific function, layered-structure nanocarbons, including graphene oxide (GO), reduced GO (rGO), and graphitic carbon nitride (g-C3N4), show potential activity as metal-free catalysts in heterogeneous catalytic ozonation for water purification. In this study, layered-structure nanocarbons GO, rGO, and g-C3N4 were applied as metal-free catalysts in catalytic ozonation to investigate the mechanism and driving force of reaction oxygen species formation. Although GO showed excellent catalytic activity, its instability was a decisive factor in its catalytic ozonation mechanism, due to the layered structure and chemical properties destroyed by ozone and formed free radicals. Meanwhile, the structure of rGO was preserved in catalytic ozonation, enabling a stable and kinetics-enhanced catalytic reaction. Interestingly, g-C3N4 showed activity in catalytic ozonation for refractory organic compound degradation and bromate elimination for the first time. X-ray photoelectron spectroscopy and in-situ electron paramagnetic resonance spectra showed that surface oxygen-containing functional groups (such as -OH, -C=O, and -COOH) in layered-structure nanocarbons were sequentially reduced either by direct oxidation or by promoting ozone decomposition to form free radicals and H2O2. The original inherent delocalized electrons generated by electron-rich nitrogen vacancies in g-C3N4 promoted ozone decomposition to generate hydroxyl radicals. Through systematic study, new insights into the catalytic ozonation processes of GO, rGO, and g-C3N4 were evaluated and explained. This work presents an extensive investigation into catalytic ozonation using layered-structured nanocarbons, which will be important for the design of nanocarbons-based catalysts and improve understanding of the principles of heterogeneous catalytic ozonation.
机翻摘要
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关键词/主题词
Bromate elimination;Catalytic ozonation;Electron transfer;Layered-structure nanocarbons;Reactive oxygen species;
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