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Engineering Electron-Rich Sites on CoSe2-x Nanosheets for the Enhanced Electroanalysis of As(III): A Study on the Electronic Structure via X-ray Absorption Fine Structure Spectroscopy and Density Functional Theory Calculation
Chen, Shi-Hua1,2; Song, Zong-Yin1,2; Xiao, Xiang-Yu1,2; Huang, Hong-Qi3,4; Yang, Yuan-Fan1,2; Li, Pei-Hua1; Yang, Meng1; Huang, Xing-Jiu1,2
2022-02-01
Source PublicationANALYTICAL CHEMISTRY
ISSN0003-2700
Corresponding AuthorLi, Pei-Hua(peihuali@issp.ac.cn) ; Yang, Meng(myang@iim.ac.cn) ; Huang, Xing-Jiu(xingjiuhuang@iim.ac.cn)
AbstractVacancy and doping engineering are promising pathways to improve the electrocatalytic ability of nanomaterials for detecting heavy metal ions. However, the effects of the electronic structure and the local coordination on the catalytic performance are still ambiguous. Herein, cubic selenium vacancyrich CoSe2 (c-CoSe2-x) and P-doped orthorhombic CoSe2-x (o-CoSe2-x vertical bar P) were designed via vacancy and doping engineering. An o-CoSe2-x vertical bar P-modified glass carbon electrode (o-CoSe2-x vertical bar P/GCE) acquired a high sensitivity of 1.11 mu A ppb(-1) toward As(III), which is about 40 times higher than that of c-CoSe2-x, outperforming most of the reported nanomaterial-modified glass carbon electrodes. Besides, o-CoSe2-x vertical bar P/GCE displayed good selectivity toward As(III) compared with other divalent heavy metal cations, which also exhibited excellent stability, repeatability, and practicality. Xray absorption fine structure spectroscopy and density functional theory calculation demonstrate that electrons transferred from Co and Se to P sites through Co-P and Se-P bonds in o-CoSe2-x vertical bar P. P sites obtained plentiful electrons to form active centers, which also had a strong orbital coupling with As(III). In the detection process, As(III) was bonded with P and reduced by the electron-rich sites in o-CoSe2-x vertical bar P, thus acquiring a reinforced electrochemical sensitivity. This work provides an in-depth understanding of the influence of the intrinsic physicochemical properties of sensitive materials on the behavior of electroanalysis, thus offering a direct guideline for creating active sites on sensing interfaces.
DOI10.1021/acs.analchem.1c04785
WOS KeywordANODIC-STRIPPING VOLTAMMETRY
Indexed BySCI
Language英语
Funding ProjectNational Natural Science Foundation of China[21735005] ; National Natural Science Foundation of China[U1932119] ; Natural Science Foundation of Anhui Province[2008085QB79] ; China National Post-doctoral Program for Innovative Talents[BX2021317] ; China Postdoctoral Science Foundation[2019M652220] ; National Key Basic Research Program of China[2017YFA0403402] ; CASHIPS Director's Fund[YZJJ2022QN26]
Funding OrganizationNational Natural Science Foundation of China ; Natural Science Foundation of Anhui Province ; China National Post-doctoral Program for Innovative Talents ; China Postdoctoral Science Foundation ; National Key Basic Research Program of China ; CASHIPS Director's Fund
WOS Research AreaChemistry
WOS SubjectChemistry, Analytical
WOS IDWOS:000757792500001
PublisherAMER CHEMICAL SOC
Citation statistics
Document Type期刊论文
Identifierhttp://ir.hfcas.ac.cn:8080/handle/334002/127767
Collection中国科学院合肥物质科学研究院
Corresponding AuthorLi, Pei-Hua; Yang, Meng; Huang, Xing-Jiu
Affiliation1.Chinese Acad Sci, Inst Solid State Phys, Key Lab Environm Opt & Technol, Environm Mat & Pollut Control Lab,HFIPS, Hefei 230031, Peoples R China
2.Univ Sci & Technol China, Dept Mat Sci & Engn, Hefei 230026, Peoples R China
3.Anhui Univ, Inst Phys Sci, Hefei 230039, Peoples R China
4.Anhui Univ, Inst Informat Technol, Hefei 230039, Peoples R China
Recommended Citation
GB/T 7714
Chen, Shi-Hua,Song, Zong-Yin,Xiao, Xiang-Yu,et al. Engineering Electron-Rich Sites on CoSe2-x Nanosheets for the Enhanced Electroanalysis of As(III): A Study on the Electronic Structure via X-ray Absorption Fine Structure Spectroscopy and Density Functional Theory Calculation[J]. ANALYTICAL CHEMISTRY,2022.
APA Chen, Shi-Hua.,Song, Zong-Yin.,Xiao, Xiang-Yu.,Huang, Hong-Qi.,Yang, Yuan-Fan.,...&Huang, Xing-Jiu.(2022).Engineering Electron-Rich Sites on CoSe2-x Nanosheets for the Enhanced Electroanalysis of As(III): A Study on the Electronic Structure via X-ray Absorption Fine Structure Spectroscopy and Density Functional Theory Calculation.ANALYTICAL CHEMISTRY.
MLA Chen, Shi-Hua,et al."Engineering Electron-Rich Sites on CoSe2-x Nanosheets for the Enhanced Electroanalysis of As(III): A Study on the Electronic Structure via X-ray Absorption Fine Structure Spectroscopy and Density Functional Theory Calculation".ANALYTICAL CHEMISTRY (2022).
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