In-situ electronic structure redistribution tuning of single-atom Mn/g-C3N4 catalyst to trap atomic-scale lead(II) for highly stable and accurate electroanalysis

doi:10.1016/j.jhazmat.2022.129009

	In-situ electronic structure redistribution tuning of single-atom Mn/g-C3N4 catalyst to trap atomic-scale lead(II) for highly stable and accurate electroanalysis
	Li, Yong-Yu 1,4; Song, Zong-Yin 3,4; Xiao, Xiang-Yu 3,4; Zhang, Long-Ke 3,4; Huang, Hong-Qi 3,4; Liu, Wen-Qing 1,2; Huang, Xing-Jiu 3,4
刊名	JOURNAL OF HAZARDOUS MATERIALS
	2022-08-05
卷号	435
关键词	Mn single atom Electronic structure redistribution Valance cycles Atomic-scale Pb(II) Electroanalysis
ISSN号	0304-3894
DOI	10.1016/j.jhazmat.2022.129009
通讯作者	Liu, Wen-Qing(wqliu@aiofm.ac.cn) ; Huang, Xing-Jiu(xingjiuhuang@iim.ac.cn)
英文摘要	Constructing catalysts with simple structures, uniform effective sites, and excellent performance is crucial for understanding the reaction mechanism of target pollutants. Herein, the single-atom catalyst of Mn-intercalated graphitic carbon nitride (Mn/g-C3N4) was prepared. It was found that the intercalated Mn atoms acted as strong electron donors to effectively tune the electronic structure distribution of the in-situ N atoms, providing a large number of negative potential atomic-scale sites for catalytic reactions. In the detection, the in-situ N atom established an electron bridge for the transient electrostatic trapping of free Pb(II), which induced Pb-N-Mn coordination bonding. Even in g-C3N4-loaded Mn nanoparticles, the N atom was again confirmed to be the interaction site for coupling with Pb. And the Mn-II-N-4-C/Mn-IV-N-4-C cycle actively participated in the electrocatalysis of Pb(II) was confirmed. Moreover, Mn/g-C3N4 achieved highly stable and accurate detection for Pb(II) with a sensitivity of 2714.47 mu A.mu M-1.cm(-2). And excellent reproducibility and specific detection of real water samples made the electrode practical. This study contributes to understanding the changes in the electronic structure of chemically inert substrates after single-atom intercalation and the interaction between contaminants and the microstructure of sensitive materials, providing a guiding strategy for designing highly active electrocatalytic interfaces for accurate electroanalysis.
资助项目	Project of the National Natural Science Foundation of China[21735005] ; National Key Research and Development Program of China[2021YFB3201400] ; Natural Science Foundation of Anhui Province[2008085QB79] ; Key Research and Development Program of Anhui Province[202104i07020006] ; Key Research and Development Program of Anhui Province[202104i07020011] ; Presidential Foundation of Hefei Institutes of Physical Science, Chinese Academy of Sciences[YZJJZX202019] ; China Postdoctoral Innovation Talents Supporting Project[BX2021317]
WOS研究方向	Engineering ; Environmental Sciences & Ecology
语种	英语
出版者	ELSEVIER
WOS记录号	WOS:000799036300005
资助机构	Project of the National Natural Science Foundation of China ; National Key Research and Development Program of China ; Natural Science Foundation of Anhui Province ; Key Research and Development Program of Anhui Province ; Presidential Foundation of Hefei Institutes of Physical Science, Chinese Academy of Sciences ; China Postdoctoral Innovation Talents Supporting Project
内容类型	期刊论文
源URL	[http://ir.hfcas.ac.cn:8080/handle/334002/131131]
专题	中国科学院合肥物质科学研究院
通讯作者	Liu, Wen-Qing; Huang, Xing-Jiu
作者单位	1.Tianjin Univ, Sch Environm Sci & Engn, Tianjin 300350, Peoples R China 2.Anhui Inst Opt & Fine Mech, Chinese Acad Sci, Hefei 230031, Peoples R China 3.Univ Sci & Technol China, Dept Mat Sci & Engn, Hefei 230026, Peoples R China 4.Inst Solid State Phys, Chinese Acad Sci, Key Lab Environm Opt & Technol, Environm Mat & Pollut Control Lab, Hefei 230031, Peoples R China
推荐引用方式 GB/T 7714	Li, Yong-Yu,Song, Zong-Yin,Xiao, Xiang-Yu,et al. In-situ electronic structure redistribution tuning of single-atom Mn/g-C3N4 catalyst to trap atomic-scale lead(II) for highly stable and accurate electroanalysis[J]. JOURNAL OF HAZARDOUS MATERIALS,2022,435.
APA	Li, Yong-Yu.,Song, Zong-Yin.,Xiao, Xiang-Yu.,Zhang, Long-Ke.,Huang, Hong-Qi.,...&Huang, Xing-Jiu.(2022).In-situ electronic structure redistribution tuning of single-atom Mn/g-C3N4 catalyst to trap atomic-scale lead(II) for highly stable and accurate electroanalysis.JOURNAL OF HAZARDOUS MATERIALS,435.
MLA	Li, Yong-Yu,et al."In-situ electronic structure redistribution tuning of single-atom Mn/g-C3N4 catalyst to trap atomic-scale lead(II) for highly stable and accurate electroanalysis".JOURNAL OF HAZARDOUS MATERIALS 435(2022).