Journal
JOURNAL OF POWER SOURCES
Volume 363, Issue -, Pages 260-268Publisher
ELSEVIER
DOI: 10.1016/j.jpowsour.2017.07.107
Keywords
Co,N-codoped graphene; 3D graphene; Hydrogen evolution reaction; Active centre; Electrocatalyst
Funding
- Natural Science Foundation of Jiangsu Province, China [BK20161191]
- National Natural Science Foundation of China [2147603]
- Advanced Catalysis and Green Manufacturing Collaborative Innovation Center of Jiangsu Province
- National Science Foundation [TG-DMR140083]
- National Energy Research Scientific Computing Center (NERSC)
- Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]
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Co and N co-doped carbon (CNC) material is one of the most promising precious-metal-free catalyst for hydrogen evolution reaction (HER), however, widespread application of CNC will require continuous innovation and optimization of fabrication to maximize electrocatalytic performance, which is always a challenge. Herein, two types of three-dimensional (3D) graphene materials synthesized by one-step of simultaneous doping (Co,N/3DG-1) and two-step of sequential doping (Co,N/3DG-2) respectively, are evaluated and correlated their electrocatalytic activity for HER with experimental parameters. The results indicate that Co,N/3DG-2 exhibits significantly better electrocatalytic activity than Co,N/3DG-1. The structure analysis reveals that Co,N/3DG-2 has more moderate Co-N coordinated number than Co,N/3DG-1. Density functional theory calculations unravels that the equilibrium C and N around Co atom is more favorable to the adsorption and desorption of hydrogen. The results shed new light on the rational design of dual hetero-atom co-doped carbon materials, which may be applicable to other energy conversion and storage systems. (C) 2017 Elsevier B.V. All rights reserved.
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