Zhu Yuanzhi, Yang Xiaoxuan, Peng Cheng, Priest Cameron, Mei Yi, Wu Gang
Faculty of Chemical Engineering, Yunnan Provincial Key Laboratory of Energy Saving in Phosphorus Chemical Engineering and New Phosphorus Materials, Kunming University of Science and Technology, Kunming, 650500, China.
Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY, 14260, USA.
Small. 2021 Apr;17(16):e2005148. doi: 10.1002/smll.202005148. Epub 2021 Jan 15.
The electrochemical CO reduction reaction (CO RR) is a promising strategy to achieve electrical-to-chemical energy storage while closing the global carbon cycle. The carbon-supported single-atom catalysts (SACs) have great potential for electrochemical CO RR due to their high efficiency and low cost. The metal centers' performance is related to the local coordination environment and the long-range electronic intercalation from the carbon substrates. This review summarizes the recent progress on the synthesis of carbon-supported SACs and their application toward electrocatalytic CO reduction to CO and other C and C products. Several SACs are involved, including MN catalysts, heterogeneous molecular catalysts, and the covalent organic framework (COF) based SACs. The controllable synthesis methods for anchoring single-atom sites on different carbon supports are introduced, focusing on the influence that precursors and synthetic conditions have on the final structure of SACs. For the CO RR performance, the intrinsic activity difference of various metal centers and the corresponding activity enhancement strategies via the modulation of the metal centers' electronic structure are systematically summarized, which may help promote the rational design of active and selective SACs for CO reduction to CO and beyond.
电化学CO还原反应（CO RR）是一种很有前景的策略，可实现电能到化学能的存储，同时闭合全球碳循环。碳负载单原子催化剂（SACs）因其高效率和低成本，在电化学CO RR方面具有巨大潜力。金属中心的性能与局部配位环境以及来自碳基底的长程电子嵌入有关。本文综述了碳负载SACs合成及其在电催化CO还原为CO以及其他含碳产物方面应用的最新进展。涉及了几种SACs，包括MN催化剂、多相分子催化剂以及基于共价有机框架（COF）的SACs。介绍了在不同碳载体上锚定单原子位点的可控合成方法，重点关注前驱体和合成条件对SACs最终结构的影响。对于CO RR性能，系统总结了各种金属中心的本征活性差异以及通过调节金属中心电子结构实现的相应活性增强策略，这可能有助于推动用于将CO还原为CO及其他产物的活性和选择性SACs的合理设计。
