期刊
INTERNATIONAL JOURNAL OF ENERGY RESEARCH
卷 46, 期 2, 页码 1032-1042出版社
WILEY-HINDAWI
DOI: 10.1002/er.7222
关键词
electrocatalytical mechanism; first-principles calculation; graphene; oxygen reduction reaction; single-atom catalyst
资金
- Ministry of Science and Technology, Taiwan [MOST 107-2113-M-033-004, MOST 108-2113-M-033-001, MOST 109-2113-M-033-001]
The study investigated the electrocatalytic mechanisms of transition metal atom-doped graphene for the oxygen reduction reaction, revealing different pathways based on the structures of intermediates. The overpotential of ORR was predicted with Pd@sv-graphene showing the best activity among the catalysts.
The extension of low-expense and stable electrocatalysts for oxygen reduction reaction (ORR) is of importance to improve the performance of metal-air batteries and fuel cells. In this work, we unravel the ORR electrocatalytical mechanisms on a series of transition metal atom-doped on the defect graphene (TM@sv-graphene) by carrying out spin-polarized first-principles computations. The formation energy of the TM@sv-graphene, which is related to its stability, along with the binding energy of O-2, OOH, 2OH, OH, and O species are evaluated. The calculations of Gibbs free energy show that two different pathways, O* mechanism and 2OH* mechanism, of ORR compete with each other based on the structures of intermediates (OOH, 2OH, OH and O). It is found that Co, Rh, Ir, Pt, and Mn@sv-graphene favor the O* mechanism while Ag, Au, Cd, Cu, Zn, Fe, Ni, Pd, Sc, Cr, Ti, Zr, and V@sv-graphene strongly promote the 2OH* mechanism. The overpotential (eta) of the ORR is predicted and can be a valid descriptor that manifests the catalytic activity of different TM@sv-graphene. Among these catalysts, the Pd@sv-graphene (eta = 1.20 V) exhibits the best activity for the ORR. The results provide new insight into electrochemical mechanism of ORR for novel single-atom electrocatalyst.
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