Density functional theory study of active sites on nitrogen-doped graphene for oxygen reduction reaction

• Published in: Royal Society open science Vol. 8; no. 9; p. 210272
• Main Authors: Yan, Ping, Shu, Song, Zou, Longhua, Liu, Yongjun, Li, Jianjun, Wei, Fusheng
• Format: Journal Article
• Language: English
• Published: England The Royal Society 01.09.2021
• Subjects: Chemistry; density functional theory; graphene; mechanism; N-doped; oxygen reduction reaction; N-doped; mechanism; oxygen reduction reaction; graphene; density functional theory
• ISSN: 2054-5703; 2054-5703
• DOI: 10.1098/rsos.210272

Oxygen reduction reaction (ORR) remains challenging due to its complexity and slow kinetics. In particular, Pt-based catalysts which possess outstanding ORR activity are limited in application with high cost and ease of poisoning. In recent years, nitrogen-doped graphene has been widely studied as a potential ORR catalyst for replacing Pt. However, the vague understanding of the reaction mechanism and active sites limits the potential ORR activity of nitrogen-doped graphene materials. Herein, density functional theory is used to study the reaction mechanism and active sites of nitrogen-doped graphene for ORR at the atomic level, focusing on explaining the important role of nitrogen species on ORR. The results reveal that graphitic N (GrN) doping is beneficial to improve the ORR performance of graphene, and dual-GrN-doped graphene can demonstrate the highest catalytic properties with the lowest barriers of ORR. These results provide a theoretical guide for designing catalysts with ideal ORR property, which puts forward a new approach to conceive brilliant catalysts related to energy conversion and environmental catalysis.