Ultra-Sensitive and Selective Detection of Arsenic(III) via Electroanalysis over Cobalt Single-Atom Catalysts

doi:10.1021/acs.analchem.0c00677

	Ultra-Sensitive and Selective Detection of Arsenic(III) via Electroanalysis over Cobalt Single-Atom Catalysts
	Li, Pei-Hua 1,2,3; Yang, Meng 1,2; Li, Yi-Xiang 1,2; Song, Zong-Yin 1,2; Liu, Jin-Huai 1,2; Lin, Chu-Hong 1,2; Zeng, Jie 3; Huang, Xing-Jiu 1,2
刊名	ANALYTICAL CHEMISTRY
	2020-04-21
卷号	92
ISSN号	0003-2700
DOI	10.1021/acs.analchem.0c00677
通讯作者	Yang, 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)
英文摘要	Achieving 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.
资助项目	National 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
WOS关键词	CO OXIDATION ; IDENTIFICATION ; SITES ; WATER
WOS研究方向	Chemistry
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000527779200065
资助机构	National 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
内容类型	期刊论文
源URL	[http://ir.hfcas.ac.cn:8080/handle/334002/103395]
专题	中国科学院合肥物质科学研究院
通讯作者	Yang, Meng; Lin, Chu-Hong; Zeng, Jie; Huang, Xing-Jiu
作者单位	1.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
推荐引用方式 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).