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Nano Research

Article Title

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

Authors

Linzhong Wu, Institute of Functional Nano & Soft Materials , 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
Mingyu Chu, Institute of Functional Nano & Soft Materials , Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices, Soochow University, No. 199 Ren’ai Road, Suzhou 215123, China
Jin Gong, Institute of Functional Nano & Soft Materials , Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices, Soochow University, No. 199 Ren’ai Road, Suzhou 215123, China
Muhan Cao, Institute of Functional Nano & Soft Materials , Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices, Soochow University, No. 199 Ren’ai Road, Suzhou 215123, China
Yu Liu, Institute of Functional Nano & Soft Materials , Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices, Soochow University, No. 199 Ren’ai Road, Suzhou 215123, China
Yong Xu, Institute of Functional Nano & Soft Materials , 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

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.

Publisher

Tsinghua University Press

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