New Insights into the Generation of Singlet Oxygen in the Metal-Free Peroxymonosulfate Activation Process: Important Role of Electron-Deficient Carbon Atoms
文献类型:期刊论文
作者 | Gao, Yaowen; Chen, Zhenhuan; Zhu, Yue; Li, Tong; Hu, Chun |
刊名 | ENVIRONMENTAL SCIENCE & TECHNOLOGY
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出版日期 | 2020-01-21 |
卷号 | 54期号:2页码:1232-1241 |
ISSN号 | 0013-936X |
英文摘要 | A nonradical oxidation process via metal-free peroxymonosulfate (PMS) activation has recently attracted considerable attention for organic pollutant degradation; however, the origin of singlet oxygen (O-1(2)) generation still remains controversial. In this study, nitrogen-doped carbon nanosheets (NCN-900) derived from graphitic carbon nitride were developed for activation of PMS and elucidation of O-1(2) production. With a large specific surface area (1218.7 m(2) g(-1)) and high nitrogen content (14.5 at %), NCN-900 exhibits superior catalytic activity in PMS activation, as evidenced by complete degradation of bisphenol A within 2 min using 0.1 g L-1 NCN-900 and 2 mM PMS. Moreover, the reaction rate constant fitted by pseudo-first-order kinetics for NCN-900 reaches an impressive value of 3.1 min(-1). Electron paramagnetic resonance measurements and quenching tests verified O-1(2) as the primary reactive oxygen 900/PMS system. Based on X-ray photoelectron spectroscopy analysis and theoretical calculations, an unexpected generation pathway of O-1(2) involving PMS oxidation over the electron-deficient carbon atoms neighboring graphitic N in NCN-900 was unraveled. Besides, the NCN-900/PMS system is also applicable for remediation of actual industrial wastewater. This work highlights the important role of electron-deficient carbon atoms in O-1(2) generation from PMS oxidation and furnishes theoretical support for further relevant studies. |
源URL | [http://ir.rcees.ac.cn/handle/311016/45333] ![]() |
专题 | 生态环境研究中心_中国科学院饮用水科学与技术重点实验室 |
推荐引用方式 GB/T 7714 | Gao, Yaowen,Chen, Zhenhuan,Zhu, Yue,et al. New Insights into the Generation of Singlet Oxygen in the Metal-Free Peroxymonosulfate Activation Process: Important Role of Electron-Deficient Carbon Atoms[J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY,2020,54(2):1232-1241. |
APA | Gao, Yaowen,Chen, Zhenhuan,Zhu, Yue,Li, Tong,&Hu, Chun.(2020).New Insights into the Generation of Singlet Oxygen in the Metal-Free Peroxymonosulfate Activation Process: Important Role of Electron-Deficient Carbon Atoms.ENVIRONMENTAL SCIENCE & TECHNOLOGY,54(2),1232-1241. |
MLA | Gao, Yaowen,et al."New Insights into the Generation of Singlet Oxygen in the Metal-Free Peroxymonosulfate Activation Process: Important Role of Electron-Deficient Carbon Atoms".ENVIRONMENTAL SCIENCE & TECHNOLOGY 54.2(2020):1232-1241. |
入库方式: OAI收割
来源:生态环境研究中心
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