Journal
ADVANCED ENERGY MATERIALS
Volume 9, Issue 10, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.201803689
Keywords
charge transfer; density functional theory; density of states; hydrogen evolution reaction; single atom catalysts
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Funding
- Research Grant Council of Hong Kong SAR [16204815]
- NSFC-RGC Joint Research Scheme [N_HKUST607/17]
- Innovation and Technology Commission [ITC-CNERC14SC01]
- U.S.DOE [DE-AC02-06CH11357]
- Canadian Light Source
- Southern Federal University [VnGr-07/2017-08]
- School of Engineering, at HKUST
- [201704030134]
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The proper choice of nonprecious transition metals as single atom catalysts (SACs) remains unclear for designing highly efficient electrocatalysts for hydrogen evolution reaction (HER). Herein, 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 d(z)(2) 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. This systematic study gives a fundamental understanding about the design of highly efficient SACs for HER.
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