Selenium-Enriched Nickel Selenide Nanosheets as a Robust Electrocatalyst for Hydrogen Generation.
To address the urgent need for clean and sustainable energy, the rapid development of hydrogen-based technologies has started to revolutionize the use of earth-abundant noble-metal-free catalysts for the hydrogen evolution reaction (HER). Like the active sites of hydrogenases, the cation sites of pyrite-type transition-metal dichalcogenides have been suggested to be active in the HER. Herein, we synthesized electrodes based on a Se-enriched NiSe2 nanosheet array and explored the relationship between the anion sites and the improved hydrogen evolution activity through theoretical and experimental studies. The free energy for atomic hydrogen adsorption is much lower on the Se sites (0.13 eV) than on the Ni sites (0.87 eV). Notably, this electrode benefits from remarkable kinetic properties, with a small overpotential of 117 mV at 10 mA cm(-2) , a low Tafel slope of 32 mV per decade, and excellent stability. Control experiments showed that the efficient conversion of H(+) into H2 is due to the presence of an excess of selenium in the NiSe2 nanosheet surface.
CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, National Center for Nanoscience and Technology, Beijing, 100190, China.|University of Chinese Academy of Sciences, Beijing, 100049, P.R. China.
Fengmei
F
Wang
National Center for Nanoscience and Technology, Beijing, 100190, China.
Yuanchang
Y
Li
CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, National Center for Nanoscience and Technology, Beijing, 100190, China.|University of Chinese Academy of Sciences, Beijing, 100049, P.R. China.
Tofik Ahmed
TA
Shifa
CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, National Center for Nanoscience and Technology, Beijing, 100190, China.|University of Chinese Academy of Sciences, Beijing, 100049, P.R. China.
Kaili
K
Liu
CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, National Center for Nanoscience and Technology, Beijing, 100190, China.|University of Chinese Academy of Sciences, Beijing, 100049, P.R. China.
Feng
F
Wang
CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, National Center for Nanoscience and Technology, Beijing, 100190, China.
Zhenxing
Z
Wang
National Center for Nanoscience and Technology, Beijing, 100190, China.
Peng
P
Xu
National Center for Nanoscience and Technology, Beijing, 100190, China.
Qisheng
Q
Wang
CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, National Center for Nanoscience and Technology, Beijing, 100190, China. hej@nanoctr.cn.
Jun
J
He
chalcogenides; electrocatalysis; hydrogen evolution reaction; nickel; selenium