Rational Design of Graphene-Supported Single Atom Catalysts for Hydrogen Evolution Reaction

The proper choice of nonprecious transition metals as single atom catalysts (SACs) remains unclear for designing highly efficient electrocatalysts for hydrogen evolution reaction (HER). In this article, reported is an activity correlation with catalysts, electronic structure, in order to clarify the...

Full description

Saved in:
Bibliographic Details
Published in:Advanced energy materials 2019-01, Vol.9 (10)
Main Authors: Hossain, Md Delowar, Liu, Zhenjing, Zhuang, Minghao, Yan, Xingxu, Xu, Gui-Liang, Gadre, Chaitanya Avinash, Tyagi, Abhishek, Abidi, Irfan Haider, Sun, Cheng-Jun, Wong, Hoilun, Guda, Alexander, Hao, Yufeng, Pan, Xiaoqing, Amine, Khalil, Luo, Zhengtang
Format: Article
Language:English
Subjects:
charge transfer
density functional theory
density of states
hydrogen evolution reaction
INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
MATERIALS SCIENCE
single atom catalysts
Online Access:Get full text
Tags: Add Tag
No Tags, Be the first to tag this record!
Description
Summary:The proper choice of nonprecious transition metals as single atom catalysts (SACs) remains unclear for designing highly efficient electrocatalysts for hydrogen evolution reaction (HER). In this article, reported is an activity correlation with catalysts, electronic structure, in order to clarify the origin of reactivity for a series of transition metals supported on nitrogen-doped graphene as SACs for HER by a combination of density functional theory calculations and electrochemical measurements. Only few of the transition metals (e.g., Co, Cr, Fe, Rh, and V) as SACs show good catalytic activity toward HER as their Gibbs free energies are varied between the range of -0.20 to 0.30 eV but among which Co-SAC exhibits the highest electrochemical activity at 0.13 eV. Electronic structure studies show that the energy states of active valence dz2 orbitals and their resulting antibonding state determine the catalytic activity for HER. The fact that the antibonding state orbital is neither completely empty nor fully filled in the case of Co-SAC is the main reason for its ideal hydrogen adsorption energy. Moreover, the electrochemical measurement shows that Co-SAC exhibits a superior hydrogen evolution activity over Ni-SAC and W-SAC, confirming the theoretical calculation. Lastly, this systematic study gives a fundamental understanding about the design of highly efficient SACs for HER.
ISSN:1614-6832
1614-6840