Constructing Atomic-Level Defect as the Catalytic Site by Removing a Single Metal Atom from the Nanoclusters

作者：Shuang Wang, Chao Han, Xing Chen, Yifei Xiang, Qinzhen Li, Jinsong Chai, Sha Yang, Yuanxin Du, Qiquan Luo, Manzhou Zhu · 发表于：ACS Nano · 年份：2025 · DOI：10.1021/acsnano.5c06625 · 被引用次数：13 · 研究领域：Nanocluster Synthesis and Applications、Advanced Nanomaterials in Catalysis、Catalytic Processes in Materials Science

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.