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Single-Atom Mn-N-4 Site-Catalyzed Peroxone Reaction for the Efficient Production of Hydroxyl Radicals in an Acidic Solution
Guo, Zhuang1,2; Xie, Yongbin1; Xiao, Jiadong3; Zhao, Zhi-Jian4; Wang, Yuxian5; Xu, Zhaomeng1,2; Zhang, Yi1; Yin, Lichang6; Cao, Hongbin1; Gong, Jinlong4
2019-07-31
Source PublicationJOURNAL OF THE AMERICAN CHEMICAL SOCIETY
ISSN0002-7863
Volume141Issue:30Pages:12005-12010
AbstractThe 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.
DOI10.1021/jacs.9b04569
Language英语
WOS KeywordGRAPHITIC CARBON NITRIDE ; RESONANCE RAMAN ; WASTE-WATER ; OZONATION ; OXIDATION ; OZONE ; DECOMPOSITION ; PEROXIDE ; NITROGEN ; SYNERGY
Funding ProjectNational 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 Research AreaChemistry
WOS SubjectChemistry, Multidisciplinary
Funding OrganizationNational Natural Science Foundation of China ; Beijing Natural Science Foundation ; Program of Introducing Talents of Discipline to Universities
WOS IDWOS:000479018200042
PublisherAMER CHEMICAL SOC
Citation statistics
Cited Times:1[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.ipe.ac.cn/handle/122111/30560
Collection中国科学院过程工程研究所
Corresponding AuthorYin, Lichang; Cao, Hongbin; Gong, Jinlong
Affiliation1.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
Recommended Citation
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.
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