Highly Sensitive and Stable Determination of As(III) under Near-Neutral Conditions: Benefit from the Synergetic Catalysis of Pt Single Atoms and Active S Atoms over Pt-1/MoS2

doi:10.1021/acs.analchem.1c03416

	Highly Sensitive and Stable Determination of As(III) under Near-Neutral Conditions: Benefit from the Synergetic Catalysis of Pt Single Atoms and Active S Atoms over Pt-1/MoS2
	Li, Pei-Hua 1,2; Yang, Meng 1,2; Song, Zong-Yin 1,2,3; Chen, Shi-Hua 1,2,3; Xiao, Xiang-Yu 1,2,3; Lin, Chu-Hong 1,2; Huang, Xing-Jiu 1,2,3
刊名	ANALYTICAL CHEMISTRY
	2021-11-16
卷号	93
ISSN号	0003-2700
DOI	10.1021/acs.analchem.1c03416
通讯作者	Yang, Meng(myang@iim.ac.cn) ; Lin, Chu-Hong(chlin@iim.ac.cn) ; Huang, Xing-Jiu(xingjiuhuang@iim.ac.cn)
英文摘要	Designing new catalysts with high activity and stability is crucial for the effective analysis of environmental pollutants under mild conditions. Here, we developed a superior catalyst of Pt single atoms anchored on MoS2 (Pt-1/MoS2) to catalyze the determination of As(III). A detection sensitivity of 3.31 mu A ppb(-1) was obtained in acetate buffer solution at pH 6.0, which is the highest compared with those obtained by other Pt-based nanomaterials currently reported. Pt-1/MoS2 exhibited excellent electrochemical stability during the detection process of As(III), even in the coexistence of Cu(II), Pb(II), and Hg(II). X-ray absorption fine structure spectroscopy and theoretical calculations revealed that Pt single atoms were stably fixed by four S atoms and activated the adjacent S atoms. Then, Pt and S atoms synergistically interacted with O and As atoms, respectively, and transferred some electrons to H3AsO3, which change the rate-determining step of H3AsO3 reduction and reduce reaction energy barriers, thereby promoting rapid and efficient accumulation for As(0). Compared with Pt nanoparticles, the weaker interaction between arsenic species and Pt-1/MoS2 enabled the effortless regeneration and cyclic utilization of active centers, which is more favorable for the oxidation of As(0). This work provides inspiration for developing highly efficient sensing platforms from the perspective of atomic-level catalysis and affords references to explore the detection mechanism of such contaminants.
资助项目	National Natural Science Foundation of China[21735005] ; National Natural Science Foundation of China[21802145] ; China Postdoctoral Innovation Talents Supporting Project[BX2021317] ; China Postdoctoral Innovation Talents Supporting Project[BX20180311] ; Natural Science Foundation of Anhui Province[2008085QB79] ; Special Foundation of President of HFIPS, Shanghai Large Scientific Facilities Center[YZJJ202102]
WOS关键词	TRANSFORMATION ; FERRIHYDRITE
WOS研究方向	Chemistry
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000721110000027
资助机构	National Natural Science Foundation of China ; China Postdoctoral Innovation Talents Supporting Project ; Natural Science Foundation of Anhui Province ; Special Foundation of President of HFIPS, Shanghai Large Scientific Facilities Center
内容类型	期刊论文
源URL	[http://ir.hfcas.ac.cn:8080/handle/334002/126518]
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; Huang, Xing-Jiu
作者单位	1.Chinese Acad Sci, Inst Solid State Phys, Environm Mat & Pollut Control Lab, Hefei 230031, Peoples R China 2.Chinese Acad Sci, Inst Solid State Phys, Key Lab Environm Opt & Technol, HFIPS, Hefei 230031, Peoples R China 3.Univ Sci & Technol China, Dept Mat Sci & Engn, Hefei 230026, Peoples R China
推荐引用方式 GB/T 7714	Li, Pei-Hua,Yang, Meng,Song, Zong-Yin,et al. Highly Sensitive and Stable Determination of As(III) under Near-Neutral Conditions: Benefit from the Synergetic Catalysis of Pt Single Atoms and Active S Atoms over Pt-1/MoS2[J]. ANALYTICAL CHEMISTRY,2021,93.
APA	Li, Pei-Hua.,Yang, Meng.,Song, Zong-Yin.,Chen, Shi-Hua.,Xiao, Xiang-Yu.,...&Huang, Xing-Jiu.(2021).Highly Sensitive and Stable Determination of As(III) under Near-Neutral Conditions: Benefit from the Synergetic Catalysis of Pt Single Atoms and Active S Atoms over Pt-1/MoS2.ANALYTICAL CHEMISTRY,93.
MLA	Li, Pei-Hua,et al."Highly Sensitive and Stable Determination of As(III) under Near-Neutral Conditions: Benefit from the Synergetic Catalysis of Pt Single Atoms and Active S Atoms over Pt-1/MoS2".ANALYTICAL CHEMISTRY 93(2021).