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Nano Research 2024, 17(1): 228-234 https://doi.org/10.1007/s12274-023-5538-9
Research Article | Issue | Published: 15 March 2023

Interfacial oxidized Pd species dominate catalytic hydrogenation of polar unsaturated bonds

Show Author's Information Pengyao You1,  Shaoqi Zhan2,3,  Pengpeng Ruan1,  Ruixuan Qin1,  Shiguang Mo1,  Yazhou Zhang1,  Kunlong Liu1,  Lansun Zheng1,  Nanfeng Zheng1( )
State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, and Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China
Department of Chemistry─BMC, Uppsala University, BMC Box 576, Uppsala S-751 23, Sweden
Department of Chemistry, University of Oxford, Oxford OX1 3QZ, UK
Keywords:
oxidized Pd, metal/oxide interface, constant particle size, Pd/SBA-15, acetophenone hydrogenation
Topics:
Catalyst activity
Cite this article:
You P, Zhan S, Ruan P, et al. Interfacial oxidized Pd species dominate catalytic hydrogenation of polar unsaturated bonds. Nano Research, 2024, 17(1): 228-234. https://doi.org/10.1007/s12274-023-5538-9
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Abstract Full text Electronic supplementary material About this article

The determination of catalytically active sites is crucial for the design of efficient and stable catalysts toward desired reactions. However, the complexity of supported noble metal catalysts has led to controversy over the locations of catalytically active sites (e.g., metal, support, and metal/support interface). Here we develop a structurally controllable catalyst system (Pd/SBA-15) to reveal the catalytic active sites for the selective hydrogenation of ketones to alcohol using acetophenone hydrogenation as model reaction. Systematic investigations demonstrated that unsupported Pd nanocrystals have no catalytic activity for acetophenone hydrogenation. However, oxidized Pd species were catalytically highly active for acetophenone hydrogenation. The catalytic activity decreased with the decreased oxidation state of Pd. This work provides insights into the hydrogenation mechanism of ketones but also other unsaturated compounds containing polar bonds, e.g., nitrobenzene, N-benzylidene-benzylamine, and carbon dioxide.


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About this article

Interfacial oxidized Pd species dominate catalytic hydrogenation of polar unsaturated bonds

Show Author's information Pengyao You1, Shaoqi Zhan2,3, Pengpeng Ruan1, Ruixuan Qin1, Shiguang Mo1, Yazhou Zhang1, Kunlong Liu1, Lansun Zheng1, Nanfeng Zheng1( )
State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, and Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China
Department of Chemistry─BMC, Uppsala University, BMC Box 576, Uppsala S-751 23, Sweden
Department of Chemistry, University of Oxford, Oxford OX1 3QZ, UK

Abstract

The determination of catalytically active sites is crucial for the design of efficient and stable catalysts toward desired reactions. However, the complexity of supported noble metal catalysts has led to controversy over the locations of catalytically active sites (e.g., metal, support, and metal/support interface). Here we develop a structurally controllable catalyst system (Pd/SBA-15) to reveal the catalytic active sites for the selective hydrogenation of ketones to alcohol using acetophenone hydrogenation as model reaction. Systematic investigations demonstrated that unsupported Pd nanocrystals have no catalytic activity for acetophenone hydrogenation. However, oxidized Pd species were catalytically highly active for acetophenone hydrogenation. The catalytic activity decreased with the decreased oxidation state of Pd. This work provides insights into the hydrogenation mechanism of ketones but also other unsaturated compounds containing polar bonds, e.g., nitrobenzene, N-benzylidene-benzylamine, and carbon dioxide.

Keywords: oxidized Pd, metal/oxide interface, constant particle size, Pd/SBA-15, acetophenone hydrogenation

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Publication history
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Acknowledgements

Publication history

Received: 23 November 2022
Revised: 26 January 2023
Accepted: 30 January 2023
Published: 15 March 2023
Issue date: January 2024

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 92261207, 21890752, and 22002126). N. F. Z. acknowledges support from the Tencent Foundation through the Xplorer Prize. We also thank the beamline BL14W1 (Shanghai Synchrotron Radiation Facility) for providing beam time, and the Supercomputing Center of University of Science and Technology of China for the computing resource.

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