journal article·2022-10-25

Synergistically Activated Pd Atom in Polymer-Stabilized Au23Pd1 Cluster

Shingo Hasegawa, Shinya Masuda, Shinjiro Takano, Koji Harano, Jun Kikkawa, Tatsuya Tsukuda

ACS Nano· Volume 16· Issue 10
Publisher page

Abstract

Single Pd atom doped Au23Pd1 clusters stabilized by polyvinylpyrrolidone (Au23Pd1:PVP) were selectively synthesized by kinetically controlled coreduction of the Au and Pd precursor ions. The geometric structure of Au23Pd1:PVP was investigated by density functional theory calculation, aberration-corrected transmission electron microscopy, extended X-ray absorption fine structure analysis, Fourier transform infrared spectroscopy of adsorbed CO, and hydrogenation catalysis. These results showed that Au23Pd1:PVP takes polydisperse but the same atomic arrangements as undoped Au24:PVP while exposing all the atoms including the Pd atom on the surface. Au23Pd1:PVP exhibited a significantly higher catalytic activity than Au24:PVP for the aerobic oxidation of p-substituted benzyl alcohols. The kinetic studies showed that the rate-determining step was the hydride abstraction from the α-carbon of the alkoxides for both systems. The activation energy for hydride abstraction by Au23Pd1:PVP was lower than that by Au24:PVP, indicating that the doped Pd atom acts as the active center.
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Research context

OpenAlex topics: Nanocluster Synthesis and Applications · Catalytic Processes in Materials Science · Advanced Nanomaterials in Catalysis

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Chemistry, Graduate School of Science, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo113-0033, Japan

Research Center for Advanced Measurement and Characterization, National Institute for Materials Science, 1-1 Namiki, Tsukuba, Ibaraki305-0044, Japan

Elements Strategy Initiative for Catalysts and Batteries (ESICB), Kyoto University, Katsura, Kyoto615-8520, Japan

Funding

Ministry of Education, Culture, Sports, Science and Technology · Core Research for Evolutional Science and Technology · Japan Society for the Promotion of Science

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