HFCAS OpenIR
Ultra-Sensitive and Selective Detection of Arsenic(III) via Electroanalysis over Cobalt Single-Atom Catalysts
Li, Pei-Hua1,2,3; Yang, Meng1,2; Li, Yi-Xiang1,2; Song, Zong-Yin1,2; Liu, Jin-Huai1,2; Lin, Chu-Hong1,2; Zeng, Jie3; Huang, Xing-Jiu1,2
2020-04-21
Source PublicationANALYTICAL CHEMISTRY
ISSN0003-2700
Corresponding AuthorYang, Meng(myang@iim.ac.cn) ; Lin, Chu-Hong(chlin@iim.ac.cn) ; Zeng, Jie(zengj@ustc.edu.cn) ; Huang, Xing-Jiu(xingjiuhuang@imm.ac.cn)
AbstractAchieving highly sensitive and selective detection of trace-level As(III) and clarifying the underlying mechanism is still a intractable problem. The electroanalysis of As(III) relies on the electrocatalytic ability of the sensing interface. Herein, we first adopt single-atom catalysts as the electrocatalyst in As(III) detection. Cobalt single-atoms anchored on nitrogen-doped carbon material (Co SAC) were found to have an extraordinary sensitivity of 11.44 mu A ppb(-1) with excellent stability and repeatability, which so far is the highest among non-noble metal nanomaterials. Co SAC also exhibited a superior selectivity toward As(III) compared with some bivalent heavy metal ions (HMIs). Combining X-ray absorption spectroscopy (XAFS), density functional theory (DFT) calculation, and reaction kinetics simulation, we demonstrated that Co single atoms stabilized in N2C2 support serve as active sites to catalyze H3AsO3 reduction via the formation of Co-O hybridization bond, leading to a lower energy barrier, promoting the breakage of As-O bonds. Importantly, the first electron transfer is the rate-limiting step of arsenic reduction and is found to be more favorable on Co-SAC both thermodynamically and kinetically. This work not only expands the potential applicaiton of single-atom catalysts in the detection and treatment of As(III), but also provides atomic-level catalytic insights into HMIs sensing interfaces.
DOI10.1021/acs.analchem.0c00677
WOS KeywordCO OXIDATION ; IDENTIFICATION ; SITES ; WATER
Indexed BySCI
Language英语
Funding ProjectNational Natural Science Foundation of China[21735005] ; National Natural Science Foundation of China[21802145] ; National Natural Science Foundation of China[U19A2015] ; China Postdoctoral Innovation Talents Supporting Project[BX20180311] ; China Postdoctoral Science Foundation[2019M652220] ; National Science Fund for Distinguished Young Scholars[21925204] ; Key Research Program of Frontier Sciences of the CAS[QYZDB-SSWSLH017] ; Major Program of Development Foundation of Hefei Center for Physical Science and Technology[2017FXZY002] ; USTC Research Funds of the Double First-Class Initiative[YD2340002002] ; One Hundred Person Project of the Chinese Academy of Sciences, China
Funding OrganizationNational Natural Science Foundation of China ; China Postdoctoral Innovation Talents Supporting Project ; China Postdoctoral Science Foundation ; National Science Fund for Distinguished Young Scholars ; Key Research Program of Frontier Sciences of the CAS ; Major Program of Development Foundation of Hefei Center for Physical Science and Technology ; USTC Research Funds of the Double First-Class Initiative ; One Hundred Person Project of the Chinese Academy of Sciences, China
WOS Research AreaChemistry
WOS SubjectChemistry, Analytical
WOS IDWOS:000527779200065
PublisherAMER CHEMICAL SOC
Citation statistics
Cited Times:16[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.hfcas.ac.cn:8080/handle/334002/103396
Collection中国科学院合肥物质科学研究院
Corresponding AuthorYang, Meng; Lin, Chu-Hong; Zeng, Jie; Huang, Xing-Jiu
Affiliation1.Chinese Acad Sci, Key Lab Environm Opt & Technol, Hefei 230031, Peoples R China
2.Chinese Acad Sci, Inst Intelligent Machines, Hefei 230031, Peoples R China
3.Univ Sci & Technol China, Chinese Acad Sci, Dept Chem Phys, Hefei Natl Lab Phys Sci Microscale,Key Lab Strong, Hefei 230026, Peoples R China
Recommended Citation
GB/T 7714
Li, Pei-Hua,Yang, Meng,Li, Yi-Xiang,et al. Ultra-Sensitive and Selective Detection of Arsenic(III) via Electroanalysis over Cobalt Single-Atom Catalysts[J]. ANALYTICAL CHEMISTRY,2020,92.
APA Li, Pei-Hua.,Yang, Meng.,Li, Yi-Xiang.,Song, Zong-Yin.,Liu, Jin-Huai.,...&Huang, Xing-Jiu.(2020).Ultra-Sensitive and Selective Detection of Arsenic(III) via Electroanalysis over Cobalt Single-Atom Catalysts.ANALYTICAL CHEMISTRY,92.
MLA Li, Pei-Hua,et al."Ultra-Sensitive and Selective Detection of Arsenic(III) via Electroanalysis over Cobalt Single-Atom Catalysts".ANALYTICAL CHEMISTRY 92(2020).
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