Single-Atom Mn-N-4 Site-Catalyzed Peroxone Reaction for the Efficient Production of Hydroxyl Radicals in an Acidic Solution

doi:10.1021/jacs.9b04569

IMR OpenIR

	Single-Atom Mn-N-4 Site-Catalyzed Peroxone Reaction for the Efficient Production of Hydroxyl Radicals in an Acidic Solution
	Guo, Zhuang 1,2; Xie, Yongbin 1; Xiao, Jiadong 3; Zhao, Zhi-Jian 4; Wang, Yuxian 5; Xu, Zhaomeng 1,2; Zhang, Yi 1; Yin, Lichang 6; Cao, Hongbin 1; Gong, Jinlong 4
通讯作者	Yin, Lichang(lcyin@imr.ac.cn) ; Cao, Hongbin(hbcao@ipe.ac.cn) ; Gong, Jinlong(jlgong@tju.edu.cn)
	2019-07-31
发表期刊	JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
ISSN	0002-7863
卷号	141 期号:30 页码:12005-12010
摘要	The peroxone reaction between O-3 and H2O2 has been deemed a promising technology to resolve the increasingly serious water pollution problem by virtue of the generation of superactive hydroxyl radicals ((OH)-O-center dot), but it suffers greatly from an extremely limited reaction rate constant under acidic conditions (ca. less than 0.1 M-1 s(-1) at pH 3). This article describes a heterogeneous catalyst composed of single Mn atoms anchored on graphitic carbon nitride, which effectively overcomes such a drawback by altering the reaction pathway and thus dramatically promotes (OH)-O-center dot generation in acid solution. Combined experimental and theoretical studies demonstrate Mn-N-4 as the catalytically active sites. A distinctive catalytic pathway involving HO2 center dot formation by the activation of H2O2 is found, which gets rid of the restriction of HO2- as the essential initiator in the conventional peroxone reaction. This work offers a new pathway of using a low-cost and easily accessible single-atom catalyst (SAC) and could inspire more catalytic oxidation strategies.
资助者	National Natural Science Foundation of China ; Beijing Natural Science Foundation ; Program of Introducing Talents of Discipline to Universities
DOI	10.1021/jacs.9b04569
收录类别	SCI
语种	英语
资助项目	National Natural Science Foundation of China[51425405] ; National Natural Science Foundation of China[51472249] ; National Natural Science Foundation of China[21525626] ; Beijing Natural Science Foundation[8172043] ; Program of Introducing Talents of Discipline to Universities[B06006]
WOS研究方向	Chemistry
WOS类目	Chemistry, Multidisciplinary
WOS记录号	WOS:000479018200042
出版者	AMER CHEMICAL SOC
引用统计	被引频次：249[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/321006/134926
专题	中国科学院金属研究所
通讯作者	Yin, Lichang; Cao, Hongbin; Gong, Jinlong
作者单位	1.Chinese Acad Sci, Inst Proc Engn, Natl Engn Lab Hydromet Cleaner Prod Technol, Beijing Engn Res Ctr Proc Pollut Control, Beijing 100190, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Univ Utrecht, Debye Inst Nanomat Sci, Inorgan Chem & Catalysis, Univ Weg 99, NL-3584 CG Utrecht, Netherlands 4.Tianjin Univ, Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Sch Chem Engn & Technol, Key Lab Green Chem Technol,Minist Educ, Tianjin 300072, Peoples R China 5.China Univ Petr, State Key Lab Heavy Oil Proc, 18 Fuxue Rd, Beijing 102249, Peoples R China 6.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, 72 Wenhua Rd, Shenyang 110016, Liaoning, Peoples R China
推荐引用方式 GB/T 7714	Guo, Zhuang,Xie, Yongbin,Xiao, Jiadong,et al. Single-Atom Mn-N-4 Site-Catalyzed Peroxone Reaction for the Efficient Production of Hydroxyl Radicals in an Acidic Solution[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2019,141(30):12005-12010.
APA	Guo, Zhuang.,Xie, Yongbin.,Xiao, Jiadong.,Zhao, Zhi-Jian.,Wang, Yuxian.,...&Gong, Jinlong.(2019).Single-Atom Mn-N-4 Site-Catalyzed Peroxone Reaction for the Efficient Production of Hydroxyl Radicals in an Acidic Solution.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,141(30),12005-12010.
MLA	Guo, Zhuang,et al."Single-Atom Mn-N-4 Site-Catalyzed Peroxone Reaction for the Efficient Production of Hydroxyl Radicals in an Acidic Solution".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 141.30(2019):12005-12010.