Dehydrogenation of ethane assisted by CO 2 over Y-doped ceria supported Au catalysts
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Dehydrogenation of ethane assisted by CO2 over Y‑doped ceria supported Au catalysts Qi Xie1 · Changxi Miao2 · Tianqi Lei1 · Weiming Hua1 · Yinghong Yue1 · Zi Gao1 Received: 9 September 2020 / Accepted: 19 November 2020 © Akadémiai Kiadó, Budapest, Hungary 2020
Abstract Dehydrogenation of ethane assisted by CO2 has been investigated over Au catalyst supported on Y-doped C eO2 nanorod. The catalysts were characterized by XRD, TEM, N2 adsorption, XPS, TG, H2-TPR and Raman spectroscopy. Enhanced activity can be obtained after the proper Y doping. The optimal catalyst Au/Ce0.9Y0.1 exhibits an ethane conversion of 20.9% and nearly 100% selectivity to ethylene without any evident tendency of deactivation in 50 h. The reducibility of surface oxygen species is found to play a key role in the dehydrogenation assisted by CO2, which can be improved by proper Y doping into C eO2 nanorod. The promoting effect of CO2 on activity is evident over Au/Ce0.9Y0.1 catalyst, due to the quick transformation of H2 product into H2O by the reverse water gas shift reaction. The catalyst stability is also improved by the addition of C O2, attributed to the elimination of coke by Bouduoard reaction. Keywords Ethane dehydrogenation · Au catalyst · CeO2 nanorod · Y-doping · CO2
Introduction Ethylene is a paramount building block in chemical industry, involving a great deal of reactions, such as polymerization, oxidation, alkylation, hydration, halogenation/hydrohalogenation, oligomerization and hydroformylation [1]. Thermal/catalytic cracking is the most commonly used technology for ethylene production. In spite of protracted and Electronic supplementary material The online version of this article (https://doi.org/10.1007/s1114 4-020-01910-9) contains supplementary material, which is available to authorized users. * Yinghong Yue [email protected] 1
Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200438, People’s Republic of China
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Shanghai Research Institute of Petrochemical Technology, Shanghai 201208, People’s Republic of China
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Reaction Kinetics, Mechanisms and Catalysis
unremitting optimization, this process is, however, highly energy and carbon intensive [2]. Catalytic conversion of ethane to ethylene has attracted more and more attention over the past several decades with the exploitation and utilization of natural gas and shale gas. Direct dehydrogenation is endothermic and limited by the thermodynamic equilibrium, which requires high reaction temperature to obtain acceptable ethylene yield, usually resulting in serious deactivation of the catalyst [3]. The above disadvantages can be overcome by oxidative dehydrogenation with oxygen [4]. However, overoxidation of ethane to C Ox is unavoidable, leading to a decrease in ethylene selectivity [5]. Carbon dioxide, a mild oxidant, is found preferable to oxygen. Not only can it improve the selectivity for ethylene, but also reduce coke by Bouduoard reaction a
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