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

作　　者：Linzhong Wu Mingyu Chu Jin Gong Muhan Cao Yu Liu Yong Xu 

机构地区：[1]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 [2]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

出　　处：《Nano Research》2021年第5期1559-1564,共6页纳米研究（英文版）

基　　金：This work was supported by the National Natural Science Foundation of China (Nos. 21703146 and 51802206);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),SWC for Synchrotron Radiation. Yong Xu acknowledges the financial support from Guangdong University of Technology.

摘　　要：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.

关 键 词：propyne selective hydrogenation Pd nanocubes zeolitic imidazolate frameworks core-shell nanostructures Pd carbide 

分 类 号：O64[理学—物理化学]