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

Yueqiang Cao; Xiaohu Ge; Yurou Li; Rui Si; Zhijun Sui; Jinghong Zhou; Xuezhi Duan; Xinggui Zhou

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

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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 a-Al_(2)O_(3) decreases the Pd^(0)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 C_(2)H_(4) 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.

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《工程（英文）》 |2021年第1期|P.103-110|共8页
作者
Yueqiang Cao; Xiaohu Ge; Yurou Li; Rui Si; Zhijun Sui; Jinghong Zhou; Xuezhi Duan; Xinggui Zhou;
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作者单位

State Key Laboratory of Chemical Engineering East China University of Science and Technology Shanghai 200237 China;

State Key Laboratory of Chemical Engineering East China University of Science and Technology Shanghai 200237 China;

State Key Laboratory of Chemical Engineering East China University of Science and Technology Shanghai 200237 China;

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;

State Key Laboratory of Chemical Engineering East China University of Science and Technology Shanghai 200237 China;

State Key Laboratory of Chemical Engineering East China University of Science and Technology Shanghai 200237 China;

State Key Laboratory of Chemical Engineering East China University of Science and Technology Shanghai 200237 China;

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原文格式 PDF
正文语种 chi
中图分类有机化学;
关键词
Acetylene semi-hydrogenation; Reaction kinetics; Support effects; Electronic effects; Pd local environment;

机译：乙炔半氢化;反应动力学;支持效果;电子效果;PD本地环境;

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

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