Biomass has the potential to become a sustainable precursor to industrial chemicals and transportation fuels, hence reducing the dependency of fossil fuels and petroleum derivatives. Acid catalyzed dehydration is a widely used method to produce platform chemicals such as furfural (FF), predominantly from C5 sugars, hydroxy-methyl-furfural (HMF), from C6 sugars, and levulinic acid/ethyl levulinate (LA/EL), from C5 or C6 sugars. The hydrogen content in these platform chemicals are relatively smaller than their parent sugar molecules due to the removal of water molecules, and the dehydration reactions results in the formation of chemically stable keto (-C=O) compounds (for example, removal of three water molecules from fructose and xylose gives HMF and FF, respectively). An essential transformation of these compounds to alternate fuels and desired industrial chemicals requires hydrogen; interestingly biomass is a potential source.In this paper, using first-principles approach, the reaction energetics and mechanisms for the liquid phase hydrogenation of levulinic to 2-oxo pentanoic acid, a precursor for the formation of valero-lactone is demonstrated using the following catalytic models: 1                    Shvo Catalyst (Ru-based and its Fe congener) in non-aqueous medium.2                    Novel Sn/Zr catalysts for Meervein-Ponndorf-Verley (MPV) reduction using alcohol as hydrogen donorsThese studies are performed in close collaboration with experimental studies and provide fundamental understanding of the reaction pathways and design of the catalyst.This work was supported by the U.S. Department of Energy under Contract DE-AC0206CH11357.  This material is based upon work supported as part of the Institute for Atom-efficient Chemical Transformations (IACT), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences.

Molecular level insights into the liquid phase catalytic hydrogenation of levulinic acid using quantum chemical methods

245th National Meeting (2013)

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