The Catalytic Use of Supported Gold Nanoparticles for Styrene Synthesis Via Oxidative Dehydrogenation of Ethylbenzene
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The Catalytic Use of Supported Gold Nanoparticles for Styrene Synthesis Via Oxidative Dehydrogenation of Ethylbenzene Jie Xu • Jun Huang • Yong-Mei Liu • Yong Cao • Yong-Xin Li • Kang-Nian Fan
Received: 16 August 2010 / Accepted: 8 October 2010 / Published online: 26 October 2010 Ó Springer Science+Business Media, LLC 2010
Abstract A series of supported gold catalysts have been prepared and tested as a new type of catalyst for the oxidative dehydrogenation of ethylbenzene to styrene. The effects of the supports (a-Mn2O3, Fe2O3, TiO2, Al2O3, and CeO2), preparation methods, gold loadings, and reaction conditions have been investigated. Among the catalysts tested, the Au/CeO2 sample containing a 6.0 wt% gold content prepared via a routine deposition–precipitation method exhibited the highest ethylbenzene conversion (66.9%) and remarkable styrene selectivity (91.0%). The superior catalytic performance of the Au/CeO2 catalysts can be attributed to a dramatic increase in the oxygen mobility and storage capacity of the parent CeO2 material in association with the closely contacted Au nanoparticles, which is confirmed by the TPR, total OSC, and XPS measurements. Keywords Gold Ceria Oxidative dehydrogenation (ODH) Ethylbenzene
Electronic supplementary material The online version of this article (doi:10.1007/s10562-010-0470-5) contains supplementary material, which is available to authorized users. J. Xu Y.-X. Li (&) College of Chemistry and Chemical Engineering, Changzhou University, Gehu Road 1, Changzhou, Jiangsu 213164, People’s Republic of China e-mail: [email protected] J. Huang Y.-M. Liu Y. Cao K.-N. Fan Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Fudan University, Shanghai 200433, People’s Republic of China
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1 Introduction In the past decade, catalysis by gold has emerged as one of the most intensively studied topics in chemistry. Au was historically considered to be chemically inert and hence a poor catalyst [1, 2]. However, when finely divided as small particles (B5 nm) and suitably deposited onto an oxide support [3, 4], Au could become a highly active and selective catalyst in many reactions including oxidation [5–7], hydrogenation [8], selective isomerization [9] and one-pot multistep reactions [10–12]. The outstanding catalytic ability of Au is related to the size and shape of the nanoparticles (NPs), the degree of coordinative unsaturation of the Au atoms, and the interactions between Au and the oxide support [2–4]. Of particular interest to the current chemical community is the Au-catalyzed selective oxidation, which is believed to be essential for the development of new alternative and greener routes toward sustainability [7, 13]. One recent focus in this area is to expand the scope of the selective aerobic oxidations [5–7] that can be efficiently catalyzed by supported Au NPs. In this context, several liquid phase aerobic oxidations, including the selective oxidation of alcohols [13–16], aldehydes [17], amines [12, 18, 19], oximes [2
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