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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
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| 2022-02-01 | |
| Source Publication | ANALYTICAL CHEMISTRY
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| ISSN | 0003-2700 |
| Corresponding Author | Li, Pei-Hua(peihuali@issp.ac.cn) ; Yang, Meng(myang@iim.ac.cn) ; Huang, Xing-Jiu(xingjiuhuang@iim.ac.cn) |
| Abstract | Vacancy 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. |
| DOI | 10.1021/acs.analchem.1c04785 |
| WOS Keyword | ANODIC-STRIPPING VOLTAMMETRY |
| Indexed By | SCI |
| Language | 英语 |
| Funding Project | National 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 Organization | National 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 Area | Chemistry |
| WOS Subject | Chemistry, Analytical |
| WOS ID | WOS:000757792500001 |
| Publisher | AMER CHEMICAL SOC |
| Citation statistics | |
| Document Type | 期刊论文 |
| Identifier | http://ir.hfcas.ac.cn:8080/handle/334002/127767 |
| Collection | 中国科学院合肥物质科学研究院 |
| Corresponding Author | Li, Pei-Hua; Yang, Meng; Huang, Xing-Jiu |
| Affiliation | 1.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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