Structural and Kinetics Understanding of Support Effects in Pd-Catalyzed Semi-Hydrogenation of Acetylene

Engineering

Xinggui Zhou¹  Rui Si²  Jinghong Zhou³  Xiaohu Ge³  Yueqiang Cao³  Yurou Li³  Zhijun Sui³  Xuezhi Duan³ 

[1] Corresponding author.;Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201800, China;State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China;

关键词: Acetylene semi-hydrogenation;    Reaction kinetics;    Support effects;    Electronic effects;    Pd local environment;   

DOI  :  

来源: DOAJ

【 摘 要 】

In this study, the support effects on the Pd-catalyzed semi-hydrogenation of acetylene have been investigated from the structural and kinetic perspectives. According to the results of kinetic analysis and X-ray photoelectron spectroscopy, hydrogen temperature-programmed reduction, temperature-programmed hydride decomposition, and in situ X-ray diffraction measurements, using carbon nanotubes as support for Pd nanocatalysts with various sizes instead of α-Al2O3 decreases the Pd0 3d binding energy and suppresses the formation of undesirable palladium hydride species, thus increasing the ethylene yield. Furthermore, X-ray absorption spectroscopy, high-resolution transmission electron microscopy, and C2H4 temperature-programmed desorption studies combined with density-functional theory calculations reveal the existence of a unique Pd local environment, containing subsurface carbon atoms, that produces positive geometric effects on the acetylene conversion reaction. Therefore, tailoring the Pd local environment and electronic properties represents an effective strategy for the fabrication and design of highly active and selective Pd semi-hydrogenation catalysts.

【 授权许可】

Unknown