Experimental and theoretical investigation of the control and balance of active sites on oxygen plasma-functionalized MoSe 2 nanosheets for efficient hydrogen evolution reaction

doi:10.1016/j.apcatb.2021.119983

	Experimental and theoretical investigation of the control and balance of active sites on oxygen plasma-functionalized MoSe 2 nanosheets for efficient hydrogen evolution reaction
	Xiao, Dezhi 3,4; Bao, De-Liang 1,5,6; Liang, Xiongyi 3,4; Wang, Ying 3,4; Shen, Jie 2; Cheng, Cheng 2; Chu, Paul K.3,4
刊名	APPLIED CATALYSIS B-ENVIRONMENTAL
	2021-07-05
卷号	288
关键词	Plasma functionalization Oxygen doping Ion energy and flux Molecular dynamics calculation Hydrogen evolution reaction
ISSN号	0926-3373
DOI	10.1016/j.apcatb.2021.119983
通讯作者	Chu, Paul K.(paul.chu@cityu.edu.hk)
英文摘要	Plasma functionalization is an effective method to improve the electrocatalytic activity of catalysts for the hydrogen evolution reaction (HER), but the relationship between the plasma and catalytic activity is not clear. Herein, oxygen plasma processing is conducted on MoSe2 nanosheets and the effects of the plasma parameters including ion energy and radical flux are investigated by plasma simulation and molecular dynamics (MD) to fathom the interactions between the plasma and catalyst. A moderate ion energy and flux produce doping effects leading to proper replacement of Se sites by oxygen atoms to balance vacancy generation. Consequently, the HER characteristics are improved as exemplified by a small overpotential of 165 mV at 10 mA cm(-2) and Tafel slope of 55.2 mV dec(-1). Based on first-principles density-functional theory calculation, increased polarization and state density distributions close to the Femi level introduced by oxygen and vacancies reduce the bandgap and Delta G(H) at the Mo, Se, and O sites, consequently enhancing charge transfer between the catalyst and electrolyte. The results convey new fundamental knowledge about plasma surface functionalization of electrochemical catalysts and enable precise and optimal selection of plasma processing parameters to control and balance the active sites for efficient water splitting.
资助项目	Hong Kong Scholars Program[XJ2018009] ; City University of Hong Kong Strategic Research Grant (SRG)[7005505]
WOS研究方向	Chemistry ; Engineering
语种	英语
出版者	ELSEVIER
WOS记录号	WOS:000627586500001
资助机构	Hong Kong Scholars Program ; City University of Hong Kong Strategic Research Grant (SRG)
内容类型	期刊论文
源URL	[http://ir.hfcas.ac.cn:8080/handle/334002/120915]
专题	中国科学院合肥物质科学研究院
通讯作者	Chu, Paul K.
作者单位	1.Vanderbilt Univ, Dept Phys & Astron, Nashville, TN 37235 USA 2.Chinese Acad Sci, Inst Plasma Phys, Hefei 230031, Peoples R China 3.City Univ Hong Kong, Dept Mat Sci & Engn, Dept Phys, Kowloon, Tat Chee Ave, Hong Kong, Peoples R China 4.City Univ Hong Kong, Dept Biomed Engn, Kowloon, Tat Chee Ave, Hong Kong, Peoples R China 5.Chinese Acad Sci, Inst Phys, Beijing 100190, Peoples R China 6.Chinese Acad Sci, Univ Chinese Acad Sci, Beijing 100190, Peoples R China
推荐引用方式 GB/T 7714	Xiao, Dezhi,Bao, De-Liang,Liang, Xiongyi,et al. Experimental and theoretical investigation of the control and balance of active sites on oxygen plasma-functionalized MoSe 2 nanosheets for efficient hydrogen evolution reaction[J]. APPLIED CATALYSIS B-ENVIRONMENTAL,2021,288.
APA	Xiao, Dezhi.,Bao, De-Liang.,Liang, Xiongyi.,Wang, Ying.,Shen, Jie.,...&Chu, Paul K..(2021).Experimental and theoretical investigation of the control and balance of active sites on oxygen plasma-functionalized MoSe 2 nanosheets for efficient hydrogen evolution reaction.APPLIED CATALYSIS B-ENVIRONMENTAL,288.
MLA	Xiao, Dezhi,et al."Experimental and theoretical investigation of the control and balance of active sites on oxygen plasma-functionalized MoSe 2 nanosheets for efficient hydrogen evolution reaction".APPLIED CATALYSIS B-ENVIRONMENTAL 288(2021).