The mechanism of hydrogen adsorption on transition metal dichalcogenides as hydrogen evolution reaction catalyst
Top Cited Papers
- 15 March 2017
- journal article
- research article
- Published by Royal Society of Chemistry (RSC) in Physical Chemistry Chemical Physics
- Vol. 19 (15), 10125-10132
- https://doi.org/10.1039/c7cp00636e
Abstract
Two-dimensional transition metal dichalcogenides (TMDs) have been widely considered as potential hydrogen evolution reaction (HER) catalysts because of their low cost and good electrochemical stability in acid conditions. The mechanism of hydrogen adsorption on TMDs plays an important role in optimizing HER activity. In this research, a series of TMDs (MX2, M = Co, Cr, Fe, Mn, Mo, Nb, Ni, Re, Sc, Tc, Ti, V, W, Zr, and X = S, Se, Te) in 2H- and 1T-phases were investigated using density functional theory to determine the relationship between hydrogen adsorption free energy (ΔGH) and electronic structure using a simple descriptor. The results showed a positive linear relation between ΔGH and the work required of the H electron to fill the unoccupied electronic states of the TMDs. Based on such linear relationships, the various defects (B-, C-, N-, O-, F-, P-, Se-doping and S-vacancy) were used to activate the inert basal planes of the 2H-phase molybdenum disulfide, which can introduce impurity states in the lower energy level to effectively accommodate the H electron. Furthermore, HER activity can be further optimized with the increasing concentration of the defects. These findings provide a practicable map of the HER performances, as well as indicating an appropriate direction for optimizing HER activity.Keywords
Funding Information
- National Natural Science Foundation of China (51302097, 51571096)
This publication has 59 references indexed in Scilit:
- Enhanced catalytic activity in strained chemically exfoliated WS2 nanosheets for hydrogen evolutionNature Materials, 2013
- Computational high-throughput screening of electrocatalytic materials for hydrogen evolutionNature Materials, 2006
- A Density Functional Study of the Chemical Differences between Type I and Type II MoS2-Based Structures in Hydrotreating CatalystsThe Journal of Physical Chemistry B, 2004
- Generalized Gradient Approximation Made SimplePhysical Review Letters, 1996
- Efficient iterative schemes forab initiototal-energy calculations using a plane-wave basis setPhysical Review B, 1996
- Projector augmented-wave methodPhysical Review B, 1994
- Ab initiomolecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germaniumPhysical Review B, 1994
- Photoelectrochemical Deposition of Nickel onto TiO2 Particles. Formation of Nickel Patterns without ResistsBulletin of the Chemical Society of Japan, 1994
- Special points for Brillouin-zone integrationsPhysical Review B, 1976
- Self-Consistent Equations Including Exchange and Correlation EffectsPhysical Review B, 1965