Insights into the di fference in metal -free activation of peroxymonosulfate and peroxydisulfate

CORC > 生态环境研究中心 > 中国科学院生态环境研究中心 > 中国科学院饮用水科学与技术重点实验室

	Insights into the di fference in metal -free activation of peroxymonosulfate and peroxydisulfate
	Gao, Yaowen; Zhu, Yue; Chen, Zhenhuan; Zeng, Qingyi; Hu, Chun
刊名	CHEMICAL ENGINEERING JOURNAL
	2020-08-15
卷号	394 页码:1-10
关键词	Graphitic carbon nitride N-doped porous carbon Peroxymonosulfate Peroxydisulfate Electron transfer
ISSN号	1385-8947
英文摘要	Metal-free activation of peroxymonosulfate (PMS) has been reported to be more efficient than peroxydisulfate (PDS) due to the asymmetrical structure of PMS. However, we report for the first time that the nitrogen-doped porous carbon (NC-900) templated from graphitic carbon nitride exhibits unexpectedly higher catalytic activity in the activation of PDS than PMS, as evidenced by 1.74-fold greater rate constant of NC-900/PDS (0.80 min(-1)) than that of NC-900/PMS (0.46 min(-1)). Moreover, NC-900 shows superior reactivity and stability to existing nitrogen-doped nanocarbons in persulfate activation. Experimental and theoretical results revealed that PMS activation involves PMS reduction over the electron-rich graphitic N and PMS oxidation around the electrondeficient carbon atom adjacent to graphitic N in NC-900, in which PMS oxidation is the main reaction rendering singlet oxygen (O-1(2)) the major reactive species. By contrast, PDS reduction over the electron-poor carbon atom dominates PDS activation on NC-900 for hydroxyl radical ((OH)-O-center dot) generation. The large amount of (OH)-O-center dot with stronger oxidation capability than O-1(2) contributes to the superiority of NC-900/PDS over NC-900/PMS in organic pollutant degradation. This work provides profound insights into the difference in metal-free PMS and PDS activation and presents fundamental frameworks in the design of advanced carbon-based catalysts toward sustainable environmental remediation.
内容类型	期刊论文
源URL	[http://ir.rcees.ac.cn/handle/311016/45317]
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,Zhu, Yue,Chen, Zhenhuan,et al. Insights into the di fference in metal -free activation of peroxymonosulfate and peroxydisulfate[J]. CHEMICAL ENGINEERING JOURNAL,2020,394:1-10.
APA	Gao, Yaowen,Zhu, Yue,Chen, Zhenhuan,Zeng, Qingyi,&Hu, Chun.(2020).Insights into the di fference in metal -free activation of peroxymonosulfate and peroxydisulfate.CHEMICAL ENGINEERING JOURNAL,394,1-10.
MLA	Gao, Yaowen,et al."Insights into the di fference in metal -free activation of peroxymonosulfate and peroxydisulfate".CHEMICAL ENGINEERING JOURNAL 394(2020):1-10.