Manipulating Selectivity of Hydroxyl Radical Generation by Single- Atom Catalysts in Catalytic Ozonation: Surface or Solution

doi:10.1021/acs.est.2c06836

IMR OpenIR

	Manipulating Selectivity of Hydroxyl Radical Generation by Single- Atom Catalysts in Catalytic Ozonation: Surface or Solution
	Wang, Jing 1,2; Xie, Yongbing 1; Yu, Guangfei 1; Yin, Lichang 3; Xiao, Jiadong 4; Wang, Yuxian 5; Lv, Weiguang 1,2; Sun, Zhi 1; Kim, Jae-Hong 6; Cao, Hongbin 1
通讯作者	Cao, Hongbin(hbcao@ipe.ac.cn)
	2022-11-29
发表期刊	ENVIRONMENTAL SCIENCE & TECHNOLOGY
ISSN	0013-936X
页码	10
摘要	Hydroxyl radical-dominated oxidation in catalytic ozonation is, in particular, important in water treatment scenarios for removing organic contaminants, but the mechanism about ozone-based radical oxidation processes is still unclear. Here, we prepared a series of transitional metal (Co, Mn, Ni) single-atom catalysts (SACs) anchored on graphitic carbon nitride to accelerate ozone decomposition and produce highly reactive center dot OH for oxidative destruction of a water pollutant, oxalic acid (OA). We experimentally observed that, depending on the metal type, OA oxidation occurred dominantly either in the bulk phase, which was the case for the Mn catalyst, or via a combination of the bulk phase and surface reaction, which was the case for the Co catalyst. We further performed density functional theory simulations and in situ X-ray absorption spectroscopy to propose that the ozone activation pathway differs depending on the oxygen binding energy of metal, primarily due to differential adsorption of O3 onto metal sites and differential coordination configuration of a key intermediate species, *OO, which is collectively responsible for the observed differences in oxidation mechanisms and kinetics.
关键词	single-atom catalysts hydroxyl radical transitional metals surface oxidation solution oxidation catalytic ozonation
资助者	National Natural Science Foundation of China ; State Key Laboratory of Vanadium and Titanium Resources Comprehensive Utilization
DOI	10.1021/acs.est.2c06836
收录类别	SCI
语种	英语
资助项目	National Natural Science Foundation of China[51934006] ; State Key Laboratory of Vanadium and Titanium Resources Comprehensive Utilization[2021P4FZG04A]
WOS研究方向	Engineering ; Environmental Sciences & Ecology
WOS类目	Engineering, Environmental ; Environmental Sciences
WOS记录号	WOS:000891808200001
出版者	AMER CHEMICAL SOC
引用统计	被引频次：10[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/176920
专题	中国科学院金属研究所
通讯作者	Cao, Hongbin
作者单位	1.Chinese Acad Sci, Inst Proc Engn, Chem & Chem Engn Data Ctr, Beijing 100190, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 4.Shinshu Univ, Res Initiat Supramat, Interdisciplinary Cluster Cutting Edge Res, Nagano 3808553, Japan 5.China Univ Petr, State Key Lab Heavy Oil Proc, State Key Lab Petr Pollut Control, Beijing 102249, Peoples R China 6.Yale Univ, Dept Chem & Environm Engn, New Haven, CT 06511 USA
推荐引用方式 GB/T 7714	Wang, Jing,Xie, Yongbing,Yu, Guangfei,et al. Manipulating Selectivity of Hydroxyl Radical Generation by Single- Atom Catalysts in Catalytic Ozonation: Surface or Solution[J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY,2022:10.
APA	Wang, Jing.,Xie, Yongbing.,Yu, Guangfei.,Yin, Lichang.,Xiao, Jiadong.,...&Cao, Hongbin.(2022).Manipulating Selectivity of Hydroxyl Radical Generation by Single- Atom Catalysts in Catalytic Ozonation: Surface or Solution.ENVIRONMENTAL SCIENCE & TECHNOLOGY,10.
MLA	Wang, Jing,et al."Manipulating Selectivity of Hydroxyl Radical Generation by Single- Atom Catalysts in Catalytic Ozonation: Surface or Solution".ENVIRONMENTAL SCIENCE & TECHNOLOGY (2022):10.