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

HFCAS OpenIR

	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 1,2; Bao, De-Liang 3,4,5; Liang, Xiongyi 1,2; Wang, Ying 1,2; Shen, Jie6 ; Cheng, Cheng 6; Chu, Paul K.1,2
	2021-07-05
发表期刊	APPLIED CATALYSIS B-ENVIRONMENTAL
ISSN	0926-3373
通讯作者	Chu, Paul K.(paul.chu@cityu.edu.hk)
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.
关键词	Plasma functionalization Oxygen doping Ion energy and flux Molecular dynamics calculation Hydrogen evolution reaction
DOI	10.1016/j.apcatb.2021.119983
收录类别	SCI
语种	英语
资助项目	Hong Kong Scholars Program[XJ2018009] ; City University of Hong Kong Strategic Research Grant (SRG)[7005505]
项目资助者	Hong Kong Scholars Program ; City University of Hong Kong Strategic Research Grant (SRG)
WOS研究方向	Chemistry ; Engineering
WOS类目	Chemistry, Physical ; Engineering, Environmental ; Engineering, Chemical
WOS记录号	WOS:000627586500001
出版者	ELSEVIER
引用统计	被引频次：45[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.hfcas.ac.cn:8080/handle/334002/120916
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.City Univ Hong Kong, Dept Mat Sci & Engn, Dept Phys, Kowloon, Tat Chee Ave, Hong Kong, Peoples R China 2.City Univ Hong Kong, Dept Biomed Engn, Kowloon, Tat Chee Ave, Hong Kong, Peoples R China 3.Vanderbilt Univ, Dept Phys & Astron, Nashville, TN 37235 USA 4.Chinese Acad Sci, Inst Phys, Beijing 100190, Peoples R China 5.Chinese Acad Sci, Univ Chinese Acad Sci, Beijing 100190, Peoples R China 6.Chinese Acad Sci, Inst Plasma Phys, Hefei 230031, 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).