Abstract
The hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) was performed in perfluoroalkoxy alkane capillary microreactors packed with a carbon-supported ruthenium (Ru/C) catalyst with an average particle diameter of 0.3 or 0.45 mm. The reaction was executed under an upstream gas–liquid slug flow with 1,4-dioxane as the solvent and H2 as the hydrogen donor in the gas phase. Operating conditions (i.e., flow rate and gas to liquid flow ratio, pressure, temperature and catalyst particle size) were varied in the microreactor to determine the influence of mass transfer and kinetic characteristics on the reaction performance. At 130 °C, 12 bar H2 and a weight hourly space velocity of the liquid feed (WHSV) of 3.0 gfeed/(gcat·h), 100% LA conversion and 84% GVL yield were obtained. Under the conditions tested (70–130 °C and 9–15 bar) the reaction rate was affected by mass transfer, given the notable effect of the mixture flow rate and catalyst particle size on the LA conversion and GVL yield at a certain WHSV. A microreactor model was developed by considering gas–liquid–solid mass transfer therein and the reaction kinetics estimated from the literature correlations and data. This model well describes the measured LA conversion for varying operating conditions, provided that the internal diffusion and kinetic rates were not considered rate limiting. Liquid–solid mass transfer of hydrogen towards the external catalyst surface was thus found dominant in most experiments. The developed model can aid in the further optimization of the Ru/C catalyzed levulinic acid hydrogenation in packed bed microreactors.
Highlights
Biomass is an abundantly available and renewable source of carbon with potential to replace fossil sources in the production of chemicals and fuels [1]
Under the conditions tested (70–130 °C and 9–15 bar) the reaction rate was affected by mass transfer, given the notable effect of the mixture flow rate and catalyst particle size on the levulinic acid (LA) conversion and GVL yield at a certain WHSV
The Ru supported on carbon (Ru/C) catalyzed hydrogenation of LA to GVL was performed in packed bed microreactors made of perfluoroalkoxy alkane (PFA) with H2 gas as the hydrogen donor and 1,4-dioxane as the solvent
Summary
Biomass is an abundantly available and renewable source of carbon with potential to replace fossil (petroleum) sources in the production of chemicals and fuels [1]. These merits are advantageous for hydrogenation reactions that often require high pressure operation to improve mass transfer (e.g., given low hydrogen solubility in the reaction solvent) and fine temperature control to avoid the hotspot formation in the reactor leading to runaway Solid catalysts for such reactions can be well handled in microreactors and are usually incorporated as wall-coatings or as small particles in a packed bed configuration [42,43,44]. The effect of various operating parameters in the packed bed microreactor (e.g., flow rate and ratio, temperature, pressure, catalyst particle size and concentration) on the reaction performance (in terms of the LA conversion and GVL yield) was investigated. With the developed model, directions for further reaction optimization in the microreactor could be established
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