Yan Ping, Shu Song, Zou Longhua, Liu Yongjun, Li Jianjun, Wei Fusheng
College of Architecture and Environment, Institute of New Energy and Low Carbon Technology, Sichuan University, Chengdu 610065, People's Republic of China.
National Engineering Research Center for Flue Gas Desulfurization, Sichuan University, Chengdu 610065, People's Republic of China.
R Soc Open Sci. 2021 Sep 1;8(9):210272. doi: 10.1098/rsos.210272. eCollection 2021 Sep.
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.
氧还原反应（ORR）因其复杂性和缓慢的动力学而仍然具有挑战性。特别是，具有出色ORR活性的铂基催化剂在应用中受到高成本和易中毒的限制。近年来，氮掺杂石墨烯作为一种潜在的替代铂的ORR催化剂受到了广泛研究。然而，对反应机理和活性位点的模糊认识限制了氮掺杂石墨烯材料的潜在ORR活性。在此，采用密度泛函理论在原子水平上研究氮掺杂石墨烯用于ORR的反应机理和活性位点，重点解释氮物种对ORR的重要作用。结果表明，石墨氮（GrN）掺杂有利于提高石墨烯的ORR性能，双GrN掺杂石墨烯能展现出最高的催化性能且具有最低的ORR势垒。这些结果为设计具有理想ORR性能的催化剂提供了理论指导，为构思与能量转换和环境催化相关的卓越催化剂提出了一种新方法。
