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Nano Research 2021, 14(5): 1559-1564 https://doi.org/10.1007/s12274-020-3235-5
Research Article | Issue | Published: 06 January 2021

Regulation of surface carbides on palladium nanocubes with zeolitic imidazolate frameworks for propyne selective hydrogenation

Show Author's Information Linzhong Wu1,2,§,  Mingyu Chu1,§,  Jin Gong1,  Muhan Cao1( ),  Yu Liu1,  Yong Xu1,2( )
Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices, Soochow University, No. 199 Ren’ai Road, Suzhou 215123, China
Guangzhou Key Laboratory of Low-Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy, Guangdong University of Technology, Guangzhou 510006, China
Keywords:
propyne selective hydrogenation, Pd nanocubes, zeolitic imidazolate frameworks, core-shell nanostructures, Pd carbide
Topics:
CarbidesCatalyst selectivity HydrogenationPalladium compounds
Cite this article:
Wu L, Chu M, Gong J, et al. Regulation of surface carbides on palladium nanocubes with zeolitic imidazolate frameworks for propyne selective hydrogenation. Nano Research, 2021, 14(5): 1559-1564. https://doi.org/10.1007/s12274-020-3235-5
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Abstract Full text Electronic supplementary material About this article

The selective hydrogenation of propyne to propylene has attracted great attention in chemical industry for removing trace amount of propyne for producing polymer-grade propylene. As the state-of-the-art catalyst, Pd suffers from the disadvantage of poor propylene selectivity due to the over-hydrogenation of propylene to propane. We here demonstrate that Pd nanocubes (NCs) coated by zeolitic imidazolate frameworks (i.e., Pd NCs@ZIF-8) can serve as highly active and selective catalysts for propyne selective hydrogenation (PSH). Benefitting from the unique properties and abundant groups of ZIF-8, Pd carbide (Pd-C) is formed on the surface of Pd NCs after thermal treatment, which acts the active sites for PSH to propylene. More importantly, the content of Pd-C can be precisely controlled by altering the calcination temperature without aggregation of Pd NCs and obvious changes in the framework of ZIF-8. The formation of Pd-C on Pd NCs@ZIF-8 can strongly suppress the H2 adsorption, and thus selectively catalyze propyne to propylene. Consequently, the optimized catalyst (i.e., Pd NCs@ZIF-8-100) exhibits a propylene selectivity of 96.4% at a propyne conversion of 93.3% at 35 °C and atmospheric pressure. This work may not only provide an efficient catalyst for PSH, but also shed a new light on the catalytic application of ZIFs.


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Electronic supplementary material
About this article

Regulation of surface carbides on palladium nanocubes with zeolitic imidazolate frameworks for propyne selective hydrogenation

Show Author's information Linzhong Wu1,2,§, Mingyu Chu1,§, Jin Gong1, Muhan Cao1( ), Yu Liu1, Yong Xu1,2( )
Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices, Soochow University, No. 199 Ren’ai Road, Suzhou 215123, China
Guangzhou Key Laboratory of Low-Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy, Guangdong University of Technology, Guangzhou 510006, China

Abstract

The selective hydrogenation of propyne to propylene has attracted great attention in chemical industry for removing trace amount of propyne for producing polymer-grade propylene. As the state-of-the-art catalyst, Pd suffers from the disadvantage of poor propylene selectivity due to the over-hydrogenation of propylene to propane. We here demonstrate that Pd nanocubes (NCs) coated by zeolitic imidazolate frameworks (i.e., Pd NCs@ZIF-8) can serve as highly active and selective catalysts for propyne selective hydrogenation (PSH). Benefitting from the unique properties and abundant groups of ZIF-8, Pd carbide (Pd-C) is formed on the surface of Pd NCs after thermal treatment, which acts the active sites for PSH to propylene. More importantly, the content of Pd-C can be precisely controlled by altering the calcination temperature without aggregation of Pd NCs and obvious changes in the framework of ZIF-8. The formation of Pd-C on Pd NCs@ZIF-8 can strongly suppress the H2 adsorption, and thus selectively catalyze propyne to propylene. Consequently, the optimized catalyst (i.e., Pd NCs@ZIF-8-100) exhibits a propylene selectivity of 96.4% at a propyne conversion of 93.3% at 35 °C and atmospheric pressure. This work may not only provide an efficient catalyst for PSH, but also shed a new light on the catalytic application of ZIFs.

Keywords: propyne selective hydrogenation, Pd nanocubes, zeolitic imidazolate frameworks, core-shell nanostructures, Pd carbide

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Publication history
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Acknowledgements

Publication history

Received: 05 September 2020
Revised: 09 November 2020
Accepted: 12 November 2020
Published: 06 January 2021
Issue date: May 2021

Copyright

© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 21703146 and 51802206) and Natural Science Foundation of Jiangsu Province (No. BK20180846). We also acknowledge the financial support from the 111 Project, Joint International Research Laboratory of Carbon-Based Functional Materials and Devices, Collaborative Innovation Center of Suzhou Nano Science and Technology (NANO-CIC), the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD), and SWC for Synchrotron Radiation. Yong Xu acknowledges the financial support from Guangdong University of Technology.

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