Constructing Atomic-Level Defect as the Catalytic Site by Removing a Single Metal Atom from the Nanoclusters
Shuang Wang, Chao Han, Xing Chen, Yifei Xiang, Qinzhen Li, Jinsong Chai, Sha Yang, Yuanxin Du, Qiquan Luo, Manzhou Zhu
Abstract
In this study, we realized the removal of a single gold atom on the surface of the Au 21 (AdmS) 13 S(F 3 Ph 3 P) (Au 21 for short) cluster by surface engineering and prepared Au 20 (AdmS) 14 (PhPy 2 P) (Au 20 for short) with an atomic-level defect. The structural analysis and comparison showed that the 21st gold atom is directly related to the exposure of the ninth gold atom in the core, which can be a catalytically active site. In catalytic comparison, Au 20 demonstrates more excellent catalytic activity than Au 21 in eCO 2 RR, with the current density of Au 20 being 3 times that of Au 21 at −1.3 V. The maximum FE CO of Au 20 is 92.47%, while that of Au 21 is 53.66% at −0.9 V. Finally, theoretical calculations point out that the charge transfer on the ninth gold atom is the most active for the increase in CO 2 adsorption and promotes the CO 2 reduction reaction.