School of Chemical Engineering, UNSW, Sydney, NSW, 2052, Australia.
Australian Institute for Bioengineering and Nanotechnology (AIBN), University of Queensland, Brisbane, Queensland, 4072, Australia.
Adv Mater. 2019 Mar;31(13):e1805367. doi: 10.1002/adma.201805367. Epub 2019 Jan 16.
The electrocatalytic nitrogen reduction reaction (NRR) is a promising catalytic system for N fixation in ambient conditions. Currently, metal-based catalysts are the most widely studied catalysts for electrocatalytic NRR. Unfortunately, the low selectivity and poor resistance to acids and bases, and the low Faradaic efficiency, production rate, and stability of metal-based catalysts for NRR make them uncompetitive for the synthesis of ammonia in comparison to the industrial Haber-Bosch process. Inspired by applications of carbon-based metal-free catalysts (CMFCs) for the oxygen reduction reaction (ORR) and CO reduction reaction (CO RR), the studies of these CMFCs in electrocatalytic NRR have attracted great attention in the past year. However, due to the differences in electrocatalytic NRR, there are several critical issues that need to be addressed in order to achieve rational design of advanced carbon-based metal-free electrocatalysts to improve activity, selectivity, and stability for NRR. Herein, the recent developments in the field of carbon-based metal-free NRR catalysts are presented, along with critical issues, challenges, and perspectives concerning metal-free catalysts for electrocatalytic reduction of nitrogen for synthesis of ammonia at ambient conditions.
电催化氮气还原反应(NRR)是一种在环境条件下固氮的很有前途的催化体系。目前,金属基催化剂是电催化 NRR 中研究最广泛的催化剂。然而,金属基催化剂用于 NRR 的低选择性和耐酸碱性差、法拉第效率低、产率低、稳定性差,使得它们在合成氨方面与工业 Haber-Bosch 工艺相比不具竞争力。受碳基无金属催化剂(CMFCs)在氧还原反应(ORR)和 CO 还原反应(CO RR)中应用的启发,这些 CMFCs 在电催化 NRR 中的研究在过去一年中引起了极大关注。然而,由于电催化 NRR 的差异,需要解决几个关键问题,才能实现对先进碳基无金属电催化剂的合理设计,以提高 NRR 的活性、选择性和稳定性。本文综述了碳基无金属 NRR 催化剂领域的最新进展,以及在环境条件下电催化氮气还原合成氨用无金属催化剂方面的关键问题、挑战和展望。