Catalytic Conversion of Glucose Micropyrolysis Vapors in Methane—using Isotope Labeling to Reveal Reaction Pathways
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© 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim Current biomass deoxygenation technologies require large quantities H2. Gaseous hydrogen is not a naturally-occurring raw material and is largely produced industrially via natural gas/methane steam reforming. Due to its high thermodynamic stability, direct use of methane as a hydrogen-donor for deoxygenation of complex oxygenates has not yet been demonstrated. Using catalytic pyrolysis studies performed at 700 °C with isotope labeled methane and glucose over Ni, Pt, Mo, and Ga impregnated HZSM-5 (Si/Al ratio 30), here we show that methane, in fact, could be used as a direct hydrogen donor for deoxygenation reactions. The amount of aromatic hydrocarbons produced increased primarily in the presence of Mo (125 % increase), and to a lesser degree, Pt (50 % increase), and Ni (22 % increase) impregnated HZSM-5 catalysts in a methane environment. Based on the metal present, results indicate the occurrence of distinct and concurrent reactions to various degrees: methane (steam) reforming and oxygenate dehydration reaction; independent aromatization of methane and oxygenates; and an intriguing methane oxygenate cross-coupling reaction where both hydrogen and carbon from methane ending up in resultant deoxygenated aromatic products. This technique paves way for the direct use of methane/natural gas for deoxygenation reactions critical to biorefining.
author list (cited authors)
Gunawardena, D. A., & Fernando, S. D.