Abstract
One wt% Ru/TiO2 catalysts prepared by a one-pot microwave-assisted polyol method have been shown to be highly active for Levulinic acid hydrogenation to γ-Valerolactone. Preparation temperature, microwave irradiation time and choice of Ru precursor were found to have a significant effect on catalyst activity. In the case of Ru(acac)3-derived catalysts, increasing temperature and longer irradiation times increased catalyst activity to a maximum LA conversion of 69%. Conversely, for catalysts prepared using RuCl3, shorter preparation times and lower temperatures yielded more active catalysts, with a maximum LA conversion of 67%. Catalysts prepared using either precursor were found to contain highly dispersed nanoparticles <3 nm in diameter. XPS analysis of the most and least active catalysts shows that the catalyst surface is covered in a layer of insoluble carbon with surface concentrations exceeding 40% in some cases. This can be attributed to the formation of large condensation oligomers from the reaction between the solvent, ethylene glycol and its oxidation products, as evidenced by the presence of C-O and C = O functionality on the catalyst surface.
Highlights
Biomass-derived feedstocks currently show potential as environmentally benign alternatives to fossil fuel derived chemicals, either directly as a fuel or as an intermediate for incorporation into existing commodity scale chemical processes [1]
A series of Ru/TiO2 catalysts was prepared from Ru(acac)3 at 150, 175 and 200 °C to Initially, a series of Ru/TiO2 catalysts was prepared from Ru(acac)3 at 150, 175 and 200 ◦ C to assess assess the effect of preparation temperature and time on catalyst activity for Levulinic acid (LA) hydrogenation
The catalysts catalysts were denoted in the manuscript using the following nomenclature: reductant-preparation were denoted in the manuscript using the following nomenclature: reductant-preparation temperature temperature (°C)-preparation time, e.g., Acac-200-10 was prepared using Ru(acac)3, at 200 °C for 10 (◦ C)-preparation time, e.g., Acac-200-10 was prepared using Ru(acac)3, at 200 ◦ C for 10 min
Summary
Biomass-derived feedstocks currently show potential as environmentally benign alternatives to fossil fuel derived chemicals, either directly as a fuel or as an intermediate for incorporation into existing commodity scale chemical processes [1]. LA was identified by the U.S Department of Energy in 2004 as a bio-derived platform chemical capable of incorporation into traditionally petroleum derived value chains [3]. The application of Levulinic acid derived species and the prerequisite chemical transformations have been thoroughly explored [4]. One such transformation is the hydrogenation of LA to γ-Valerolactone (GVL), schematically presented, with GVL itself being considered a viable platform molecule for the production of fuels or fuel additives [5] One such transformation is the hydrogenation of LA to γ-Valerolactone (GVL), schematically presented in Figure 1, with GVL itself being considered a viable platform molecule for the production of fuels or fuel additives [5]
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