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Selective hydrogenation of acetylene in excess ethylene is an important reaction in both fundamental study and practical application. Pd-based catalysts with high intrinsic activity are commonly employed, but usually suffer from low selectivity. Pd single-atom catalysts (SACs) usually exhibit outstanding ethylene selectivity due to the weak π-bonding ethylene adsorption. However, the preparation of high-loading and stable Pd SACs is still confronted with a great challenge. In this work, we report a simple strategy to fabricate Pd SACs by means of reducing conventional supported Pd catalysts at suitable temperatures to selectively encapsulate the co-existed Pd nanoparticles (NPs)/clusters. This is based on our new finding that single atoms only manifest strong metal–support interaction (SMSI) at higher reduction temperature than that of NPs/clusters. The derived Pd SACs (Pd1/CeO2 and Pd1/α-Fe2O3) were applied to acetylene selective hydrogenation, exhibiting much improved ethylene selectivity and high stability. This work offers a promising way to develop stable Pd SACs easily.


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Pd single-atom catalysts derived from strong metal–support interaction for selective hydrogenation of acetylene

Show Author's information Yalin Guo1,2Yangyang Li1,2Xiaorui Du3Lin Li1Qike Jiang4( )Botao Qiao1( )
CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
University of Chinese Academy of Sciences, Beijing 100049, China
Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, China
Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China

Abstract

Selective hydrogenation of acetylene in excess ethylene is an important reaction in both fundamental study and practical application. Pd-based catalysts with high intrinsic activity are commonly employed, but usually suffer from low selectivity. Pd single-atom catalysts (SACs) usually exhibit outstanding ethylene selectivity due to the weak π-bonding ethylene adsorption. However, the preparation of high-loading and stable Pd SACs is still confronted with a great challenge. In this work, we report a simple strategy to fabricate Pd SACs by means of reducing conventional supported Pd catalysts at suitable temperatures to selectively encapsulate the co-existed Pd nanoparticles (NPs)/clusters. This is based on our new finding that single atoms only manifest strong metal–support interaction (SMSI) at higher reduction temperature than that of NPs/clusters. The derived Pd SACs (Pd1/CeO2 and Pd1/α-Fe2O3) were applied to acetylene selective hydrogenation, exhibiting much improved ethylene selectivity and high stability. This work offers a promising way to develop stable Pd SACs easily.

Keywords: selective hydrogenation of acetylene, Pd single-atom catalysts (SACs), weak π-bonding ethylene adsorption, strong metal–support interaction (SMSI)

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Publication history
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Acknowledgements

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Received: 19 February 2022
Revised: 28 March 2022
Accepted: 29 March 2022
Published: 19 May 2022
Issue date: December 2022

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© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 21972135, 21961142006, and 51701201), CAS Project for Young Scientists in Basic Research (No. YSBR-022), and the National Key Research and Development Program of China (No. 2021YFA1500503).

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