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

文献类型：期刊论文

作者Guo, Zhuang4,5; Xie, Yongbin4; Xiao, Jiadong1; Zhao, Zhi-Jian6; Wang, Yuxian3; Xu, Zhaomeng4,5; Zhang, Yi4; Yin, Lichang2; Cao, Hongbin4; Gong, Jinlong6
刊名JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
出版日期2019-07-31
卷号141期号:30页码:12005-12010
ISSN号0002-7863
DOI10.1021/jacs.9b04569
通讯作者Yin, Lichang(lcyin@imr.ac.cn) ; Cao, Hongbin(hbcao@ipe.ac.cn) ; Gong, Jinlong(jlgong@tju.edu.cn)
英文摘要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
语种英语
出版者AMER CHEMICAL SOC
WOS记录号WOS:000479018200042
资助机构National Natural Science Foundation of China ; Beijing Natural Science Foundation ; Program of Introducing Talents of Discipline to Universities
源URL[http://ir.imr.ac.cn/handle/321006/134925]  
专题金属研究所_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.Univ Utrecht, Debye Inst Nanomat Sci, Inorgan Chem & Catalysis, Univ Weg 99, NL-3584 CG Utrecht, Netherlands
2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, 72 Wenhua Rd, Shenyang 110016, Liaoning, Peoples R China
3.China Univ Petr, State Key Lab Heavy Oil Proc, 18 Fuxue Rd, Beijing 102249, Peoples R China
4.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
5.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
6.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
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.

入库方式： OAI收割

来源：金属研究所

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