Density Functional Theory Calculation of Zn and N Codoped Graphene for Oxygen Reduction and Evolution Reactions

The highly efficient and low‐cost electrocatalysts are of great importance for energy conversion systems such as fuel cells, metal–air batteries, and water electrolyzers. Here, the activities of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) in zinc and nitrogen codoped graphene...

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Bibliographic Details
Published in:Advanced theory and simulations 2020-09, Vol.3 (9), p.n/a
Main Authors: Li, Yongcheng, Hu, Riming, Wan, Xin, Shang, Jia‐Xiang, Wang, Fu‐He, Shui, Jianglan
Format: Article
Language:English
Subjects:
DFT calculations
nonprecious metal catalysts
oxygen evolution reaction
oxygen reduction reaction
Zn–N–C
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Summary:The highly efficient and low‐cost electrocatalysts are of great importance for energy conversion systems such as fuel cells, metal–air batteries, and water electrolyzers. Here, the activities of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) in zinc and nitrogen codoped graphene with different zinc–nitrogen (Zn–N) coordination numbers and configurations are studied by density functional theory (DFT) calculations. The calculation results show that both Zn–N coordination numbers and structure configurations affect the activities of ORR and OER on ZnNx sites. Among all the calculated structures, ZnN4‐pyridine shows the lowest ORR overpotential of 0.61 V, whereas ZnN4‐pyrrole and ZnN4‐edge show lower OER overpotentials of 0.73 and 0.63 V, respectively. However, the other low N coordination structures of ZnNx‐pyridine/pyrrole/edge (x = 1/0/1–3) demonstrate poor activities. The electronic structure reveals that the O‐p orbital shows moderate hybridization strength with the N‐p and Zn‐d orbitals in O adsorbed ZnN4 systems thus facilitates the electrocatalytic reactions. The findings shed light on the rational design of bifunctional electrocatalysts for energy storage and conversion. The structure of ZnN4‐pyridine shows lower oxygen reduction reaction (ORR) overpotentials of 0.61 V, whereas ZnN4‐pyrrole and ZnN4‐edge show lower oxygen evolution reaction (OER) overpotentials of 0.73 and 0.63 V, respectively. However, the other low N coordination structures of ZnNx‐pyridine/pyrrole/edge (x = 1/0/1–3) demonstrate poor activities.
ISSN:2513-0390
2513-0390
DOI:10.1002/adts.202000054