二硫化钼
单层
塔菲尔方程
过渡金属
钼
电化学
分解水
催化作用
氢
铂金
材料科学
化学
无机化学
纳米技术
物理化学
电极
有机化学
冶金
光催化
作者
Yuting Luo,Shuqing Zhang,Haiyang Pan,Shujie Xiao,Zenglong Guo,Lei Tang,Usman Khan,Baofu Ding,Meng Li,Zhengyang Cai,Yüe Zhao,Wei Lv,Qingliang Feng,Xiaolong Zou,Junhao Lin,Hui‐Ming Cheng,Bilu Liu
出处
期刊:ACS Nano
[American Chemical Society]
日期:2019-12-13
卷期号:14 (1): 767-776
被引量:107
标识
DOI:10.1021/acsnano.9b07763
摘要
Large scale implementation of electrochemical water splitting for hydrogen evolution requires cheap and efficient catalysts to replace expensive platinum. Molybdenum disulfide is one of the most promising alternative catalysts but its intrinsic activity is still inferior to platinum. There is therefore a need to explore new active site origins in molybdenum disulfide with ultrafast reaction kinetics and to understand their mechanisms. Here, we report a universal cold hydrogen plasma reduction method for synthesizing different single atoms sitting on two-dimensional monolayers. In case of molybdenum disulfide, we design and identify a new 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 35.1 mV dec-1 and a turnover frequency of ~10^3 s-1 at 100 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.
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