Ding Mei, Tang Li, Ma Xiaoshuang, Song Caixia, Wang Shuxin
College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao, 266042, P. R. China.
Commun Chem. 2022 Dec 19;5(1):172. doi: 10.1038/s42004-022-00779-0.
Atomically precise nanoclusters (NCs) provide opportunities for correlating the structure and electrocatalytic properties at atomic level. Herein, we report the single-atom doping effect and ligand effect on CO electroreduction (eCORR) by comparing monogold-doped AuCu and homocopper Cu NCs protected by triphenylphosphine or/and tris(4-fluorophenyl)phosphine. Catalytic results revealed that the electronic distribution of Cu NCs is enormously contracted by doping Au atoms, entitling it to exhibit the unique inhibition of hydrogen evolution reaction. And the inductive effect of ligand strongly favors the formation of formate in eCORR. Overall, this work will provide guidance for the rational design of the copper-based catalysts in the eCORR.
原子精确的纳米团簇（NCs）为在原子水平上关联结构和电催化性能提供了机会。在此，我们通过比较由三苯基膦或/和三（4-氟苯基）膦保护的单金掺杂的AuCu和同铜Cu NCs，报道了单原子掺杂效应和配体效应对CO电还原（eCORR）的影响。催化结果表明，掺杂Au原子极大地收缩了Cu NCs的电子分布，使其表现出对析氢反应的独特抑制作用。并且配体的诱导效应强烈有利于eCORR中甲酸根的形成。总体而言，这项工作将为eCORR中铜基催化剂的合理设计提供指导。
