Research Article

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2016, 9(9): 2544–2550

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https://doi.org/10.1007/s12274-016-1140-8

Pd3 cluster catalysis: Compelling evidence from in operando spectroscopic, kinetic, and density functional theory studies

Chunlin Lv1,3, Hao Cheng2, Wei He3 (*), Muhammad Ishaq Ali Shah1, Congqiao Xu1, Xiangjian Meng1, Lei Jiao1, Shiqiang Wei2, Jun Li1, Lei Liu1,3,4 (*), and Yadong Li1,4

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1 Department of Chemistry and Collaborative Innovation Center for Nanomaterial Science and Engineering, Tsinghua University, Beijing 100084, China
2 National Synchrotron Radiation Laboratory and Collaborative Innovation Center for Nanomaterial Science and Engineering, University of Science and Technology of China, Hefei 230029, China
3 Tsinghua-Peking Center for Life Sciences, Tsinghua University, Beijing 100084, China
4 Center of Advanced Nanocatalysis (CAN) and Collaborative Innovation Center for Nanomaterial Science and Engineering, University of Science and Technology of China, Hefei 230026, China

Keywords: metal cluster catalysis,operando studies,active species,cycloisomerization,palladium
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  • Abstract
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Identification of metal cluster catalysis is a topic that is being investigated sincea long time. Here, we report a Pd3 metal cluster catalytic reaction investigated bymeans of operando studies. We discovered that atomically defined tri-nuclearpalladium (Pd3) is a surprisingly active catalyst for the cycloisomerization of2-phenylethynylaniline. Operando 1H NMR spectroscopy and X-ray extendedabsorption fine structure (EXAFS) measurements have indicated that the structuralintegrity of such a catalyst remains intact throughout the reaction, which hasalso been confirmed by an ex situ X-ray photoelectron spectroscopy (XPS) studyand catalyst recycling experiments. Kinetic data derived from operando IRspectroscopy measurements have shown that Pd3 is the active catalytic species.Density functional theory calculations have revealed a reaction pathway consistentwith the kinetic data, further supported by NMR titration and X-ray crystalstructure studies. Overall, the present study presents a clear example of metalcluster catalysis.
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Pd3 cluster catalysis: Compelling evidence from in operando spectroscopic, kinetic, and density functional theory studies. Nano Res. 2016, 9(9): 2544–2550 https://doi.org/10.1007/s12274-016-1140-8

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