Solvent effects in the hydrogenation of 2-butanone

详细信息    查看全文

• 作者：B.S. Akpa^a ; C. D&rsquo ; Agostino^a ; L.F. Gladden^a ; K. Hindle^b ; H. Manyar^b ; J. McGregor^a ; R. Li^a ; M. Neurock^c ; N. Sinha^c ; E.H. Stitt^d ; D. Weber^a ; J.A. Zeitler^a ; D.W. Rooney^b ; ^{d.rooney@qub.ac.uk}
• 关键词：Solvent effects ; Mixed solvents ; Mass transfer ; Heterogeneous catalysis ; Hydrogenation ; 2-Butanone ; Ru ; DFT
• 刊名：Journal of Catalysis
• 出版年：2012
• 出版时间：May, 2012
• 年：2012
• 卷：289
• 期：Complete
• 页码：30-41
• 全文大小：1695 K

文摘

In liquid-phase reaction systems, the role of the solvent is often limited to the simple requirement of dissolving and/or diluting substrates. However, the correct choice, either pure or mixed, can significantly influence both reaction rate and selectivity. For multi-phase heterogeneously catalysed reactions observed variations may be due to changes in mass transfer rates, reaction mechanism, reaction kinetics, adsorption properties and combinations thereof. The liquid-phase hydrogenation of 2-butanone to 2-butanol over a Ru/SiO₂ catalyst, for example, shows such complex rate behaviour when varying water/isopropyl alcohol (IPA) solvent ratios. In this paper, we outline a strategy which combines measured rate data with physical property measurements and molecular simulation in order to gain a more fundamental understanding of mixed solvent effects for this heterogeneously catalysed reaction. By combining these techniques, the observed complex behaviour of rate against water fraction is shown to be a combination of both mass transfer and chemical effects.