RuSn bimetallic catalysts for selective hydrogenation of levulinic acid to 纬-valerolactone

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• 作者：Stephanie G. Wettstein^a ; Jesse Q. Bond^a ; David Martin Alonso^a ; Hien N. Pham^b ; Abhaya K. Datye^b ; James A. Dumesic^a ; ^{dumesic@engr.wisc.edu}
• 关键词：Alkylphenol ; Biomass ; Heterogeneous catalysis ; Renewable resources ; Bimetallic
• 刊名：Applied Catalysis B ; Environmental
• 出版年：2012
• 期刊代码：4_09263373
• 类别：ce
• 出版时间：18 May, 2012
• 卷：117-118
• 期：Complete
• 页码：321-329
• 文件大小：1101 K

摘要

Carbon-supported ruthenium catalysts containing different amounts of tin were studied for the hydrogenation of levulinic acid (LA) to gamma-valerolactone (GVL) in a 2-sec-butyl-phenol (SBP) solvent. Results from reaction kinetics measurements (453 K and 35 bar H₂) showed that the Ru/C catalyst was initially more active for hydrogenation of both LA and SBP (i.e., 0.051 s^鈭? for conversion of LA to GVL), followed by continuous deactivation versus time on stream. In contrast, the catalyst containing equal amounts of Ru and Sn had a lower activity for LA to GVL conversion (0.005 s^鈭?), but displayed stable activity versus time on stream and showed 100%selectivity for hydrogenation of LA versus the SBP solvent. Increasing the amount of Sn to a 1 to 4 Ru:Sn atomic ratio creates an additional phase, 尾-Sn, that is not active for hydrogenation, leaches into the SBP solvent, and sinters under reaction conditions. Results from CO and O₂ chemisorption and electron microscopy measurements indicated that the Ru-based metal particles did not leach or sinter at reaction conditions, and that the surfaces of these particles became progressively enriched with Sn as the Sn-loading increases. In addition, Sn did not significantly leach from the catalysts when present as an intermetallic alloy with Ru, such as Ru₂Sn₃ and Ru₃Sn₇. Using LA produced from corn stover, the RuSn₄/C catalyst was stable and demonstrated that it is a promising catalyst to produce valuable chemicals and fuels from real biomass.