School of Chemistry and Molecular Biosciences, The University of Queensland, Brisbane 4072 (Australia).
School of Chemical Engineering, The University of New South Wales, Sydney, NSW 2033 (Australia).
ChemSusChem. 2015 Sep 7;8(17):2772-88. doi: 10.1002/cssc.201500373.
The origin of oxygen reduction reaction activity in metal-free N-doped carbons has been a stimulating, yet unsolved issue for the rational design of cost-effective electrocatalysts for fuel cells and metal-air batteries. At present, there are several inconsistent opinions on the materials chemistry and the mechanism of the oxygen reduction reaction (ORR) performed on this type of materials. This article provides a brief review of the current understanding of ORR processes and the history of electrocatalyst development. With special attention, the focus of the discussion is on the major contentions of the current opinions towards metal-free N-doped carbon chemistry and the arguments for the probable ORR mechanisms. By clarifying the fundamental aspects of each opinion, a converging consensus on N-doped carbon electrocatalysts can be established and thus facilitate the substantial development of large-capacity energy devices.
在为燃料电池和金属空气电池设计具有成本效益的电催化剂时,如何合理设计不含金属的 N 掺杂碳材料以提高其氧还原反应(ORR)活性,这一直是一个令人兴奋但尚未解决的问题。目前,对于该类材料的氧还原反应(ORR)的材料化学和反应机理,存在几种不一致的观点。本文简要综述了目前对 ORR 过程的认识以及电催化剂发展的历史。特别关注的是,讨论的重点是当前关于无金属 N 掺杂碳化学的主要观点的争议以及可能的 ORR 机制的论据。通过阐明每种观点的基本方面,可以就 N 掺杂碳电催化剂达成共识,从而促进大容量能源设备的实质性发展。