Wei Kunling, Pan Keheng, Qu Guangfei, Zhou Junhong
Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Yunnan, 650500, China.
Chem Asian J. 2023 Sep 1;18(17):e202300498. doi: 10.1002/asia.202300498. Epub 2023 Jul 19.
In recent years, single-atom catalysts (SACs) have received increasing attention in the field of electrochemical CO RR with their efficient atom utilization efficiency and excellent catalytic performance. However, their low metal loading and the presence of linear relationships for single active sites with simple structures possibly restrict their activity and practical applications. Active site tailoring at the atomic level is a visionary approach to break the existing limitations of SACs. This paper first briefly introduces the synthesis strategies of SACs and DACs. Then, combining previous experimental and theoretical studies, this paper introduces four optimization strategies, namely spin-state tuning engineering, axial functionalization engineering, ligand engineering, and substrate tuning engineering, for improving the catalytic performance of SACs in the electrochemical CO RR process by combining previous experimental and theoretical studies. Then it is introduced that DACs exhibit significant advantages over SACs in increasing metal atom loading, promoting the adsorption and activation of CO molecules, modulating intermediate adsorption, and promoting C-C coupling. At the end of this paper, we briefly and succinctly summarize the main challenges and application prospects of SACs and DACs in the field of electrochemical CO RR at present.
近年来，单原子催化剂（SACs）因其高效的原子利用效率和优异的催化性能，在电化学CO₂还原领域受到越来越多的关注。然而，其低金属负载量以及结构简单的单一活性位点存在的线性关系可能会限制它们的活性和实际应用。在原子水平上对活性位点进行剪裁是一种突破单原子催化剂现有局限性的前瞻性方法。本文首先简要介绍了单原子催化剂和双原子催化剂的合成策略。然后，结合以往的实验和理论研究，介绍了四种优化策略，即自旋态调控工程、轴向功能化工程、配体工程和基底调控工程，通过结合以往的实验和理论研究来提高单原子催化剂在电化学CO₂还原过程中的催化性能。接着介绍了双原子催化剂在增加金属原子负载量、促进CO分子的吸附和活化、调节中间体吸附以及促进C-C偶联方面比单原子催化剂具有显著优势。在本文结尾，我们简要且扼要地总结了目前单原子催化剂和双原子催化剂在电化学CO₂还原领域的主要挑战和应用前景。
