期刊
CHINESE JOURNAL OF CATALYSIS
卷 42, 期 2, 页码 245-250出版社
SCIENCE PRESS
DOI: 10.1016/S1872-2067(20)63659-2
关键词
Gold cluster; Structure fusion; Icosahedral unit; Oxidation of pyrrolidine; Active sites; Catalytic activity
资金
- National Natural Science Foundation of China [21773109, 91845104]
Atomically precise gold cluster catalysts have shown unexpected catalytic properties, with the fusion of icosahedral Au-13 units leading to a decrease in catalytic activity. Different fusion modes induce different effects, while the structural fusion modulates the chemical adsorption capacity and electronic properties of the clusters, affecting the observed catalytic reactivity.
Atomically precise gold cluster catalysts have emerged as a new frontier in catalysis science, owing to their unexpected catalytic properties. In this work, we explore the evolution of the catalytic activity of clusters formed by the structural fusion of icosahedral Au-13 units, namely Au-25(SR)(18), Au-38(SR)(24), and Au-25(PPh3)(10)(SC2H4Ph)(5)Cl-2, in the oxidation of pyrrolidine to gamma-butyrolactam. We demonstrate that the structural fusion of icosahedral Au-13 units, forming vertex-fused (vf), face-fused (ff), and body-fused (bf) clusters, can induce a decrease in the catalytic activity in the following order: Au-bf > Au-ff > Au-vf. The structural fusion of icosahedral Au-13 units in the clusters does not distinguish the adsorption modes of pyrrolidine over the three clusters from each other, but modulates the chemical adsorption capacity and electronic properties of the three clusters, which is likely to be the key reason for the observed changes in catalytic reactivity. Our results are expected to be extendable to study and design atomically defined catalysts with elaborate structural patterns, in order to produce desired products. (C) 2021, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
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