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Unsaturated Single Atoms on Monolayer Transition Metal Dichalcogenides for Ultrafast Hydrogen Evolution
Luo, Yuting1,2; Zhang, Shuqing1,2; Pan, Haiyang3; Xiao, Shujie4; Guo, Zenglong5; Tang, Lei1,2; Khan, Usman1,2; Ding, Bao-Fu1,2; Li, Meng6; Cai, Zhengyan1,2; Zhao, Yue3; Lv, Wei4; Feng, Qingliang6; Zou, Xiaolong1,2; Lin, Junhao5; Cheng, Hui-Ming1,2,7; Liu, Bilu1,2
Corresponding AuthorZou, Xiaolong(xlzou@sz.tsinghua.edu.cn) ; Lin, Junhao(linjh@sustech.edu.cn) ; Liu, Bilu(bilu.liu@sz.tsinghua.edu.cn)
2020
Source PublicationACS NANO
ISSN1936-0851
Volume14Issue:1Pages:767-776
AbstractLarge-scale implementation of electrochemical water splitting for hydrogen evolution requires cheap and efficient catalysts to replace expensive platinum. However, catalysts that work well at high current densities with ultrafast intrinsic activities is still the central challenge for hydrogen evolution. An ideal case is to use single atoms on monolayer two-dimensional (2D) materials, which simplifies the system and in turn benefits the mechanism study, but is a grand challenge to synthesize. Here, we report a universal cold hydrogen plasma reduction method for synthesizing different single atoms sitting on 2D monolayers. In the case of molybdenum disulfide, we design and identify a type of active site, i.e., unsaturated Mo single atoms on cogenetic monolayer molybdenum disulfide. The catalyst shows exceptional intrinsic activity with a Tafel slope of 36.4 mV dec(-1) in 0.5 M H2SO4 and superior performance at a high current density of 400 mA cm(-2) with an overpotential of similar to 260 mV, based on single flake microcell measurements. Theoretical studies indicate that coordinately unsaturated Mo single atoms sitting on molybdenum disulfide increase the bond strength between adsorbed hydrogen atoms and the substrates through hybridization, leading to fast hydrogen adsorption/desorption kinetics and superior hydrogen evolution activity. This work shines fresh light on preparing highly efficient electrocatalysts for water splitting and other electrochemical processes, as well as provides a general method to synthesize single atoms on two-dimensional monolayers.
Keyword2D materials molybdenum disulfide plasma single atom hydrogen evolution electrocatalysts
Funding OrganizationNational Natural Science Foundation of China ; Youth 1000-Talent Program of China, Guangdong Innovative and Entrepreneurial Research Team Program ; Bureau of Industry and Information Technology of Shenzhen for the 2017 Graphene Manufacturing Innovation Center Project ; Shenzhen Science and Technology Innovation Commission ; Development and Reform Commission of Shenzhen Municipality
DOI10.1021/acsnano.9b07763
Indexed BySCI
Language英语
Funding ProjectNational Natural Science Foundation of China[51722206] ; National Natural Science Foundation of China[11674150] ; National Natural Science Foundation of China[51920105002] ; National Natural Science Foundation of China[51950410577] ; Youth 1000-Talent Program of China, Guangdong Innovative and Entrepreneurial Research Team Program[2017ZT07C341] ; Youth 1000-Talent Program of China, Guangdong Innovative and Entrepreneurial Research Team Program[2016ZT06D348] ; Bureau of Industry and Information Technology of Shenzhen for the 2017 Graphene Manufacturing Innovation Center Project[201901171523] ; Shenzhen Science and Technology Innovation Commission[JCYJ20160613160524999] ; Development and Reform Commission of Shenzhen Municipality
WOS Research AreaChemistry ; Science & Technology - Other Topics ; Materials Science
WOS SubjectChemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
WOS IDWOS:000510531500067
PublisherAMER CHEMICAL SOC
Citation statistics
Cited Times:21[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.imr.ac.cn/handle/321006/137234
Collection中国科学院金属研究所
Corresponding AuthorZou, Xiaolong; Lin, Junhao; Liu, Bilu
Affiliation1.Tsinghua Univ, Shenzhen Geim Graphene Ctr SGC, TBSI, Shenzhen 518055, Peoples R China
2.Tsinghua Univ, TSIGS, Shenzhen 518055, Peoples R China
3.Southern Univ Sci & Technol, Inst Quantum Sci & Engn, Shenzhen 518055, Peoples R China
4.Tsinghua Univ, Grad Sch Shenzhen, Shenzhen 518055, Peoples R China
5.Southern Univ Sci & Technol, Dept Phys, Shenzhen 518055, Peoples R China
6.Northwestern Polytech Univ, Shaanxi Key Lab Opt Informat Technol, MOE Key Lab Mat Phys & Chem Extraordinary Conditi, Sch Sci, Xian 710072, Peoples R China
7.Chinese Acad Sci, Shenyang Natl Lab Mat Sci, Inst Met Res, Shenyang 110016, Peoples R China
Recommended Citation
GB/T 7714
Luo, Yuting,Zhang, Shuqing,Pan, Haiyang,et al. Unsaturated Single Atoms on Monolayer Transition Metal Dichalcogenides for Ultrafast Hydrogen Evolution[J]. ACS NANO,2020,14(1):767-776.
APA Luo, Yuting.,Zhang, Shuqing.,Pan, Haiyang.,Xiao, Shujie.,Guo, Zenglong.,...&Liu, Bilu.(2020).Unsaturated Single Atoms on Monolayer Transition Metal Dichalcogenides for Ultrafast Hydrogen Evolution.ACS NANO,14(1),767-776.
MLA Luo, Yuting,et al."Unsaturated Single Atoms on Monolayer Transition Metal Dichalcogenides for Ultrafast Hydrogen Evolution".ACS NANO 14.1(2020):767-776.
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