Aqueous phase hydrodeoxygenation of polyols over Pd/WO3-ZrO2: Role of Pd-WO3 interaction and hydrodeoxygenation pathway

作者:Liu, Changjun; Sun, Junming; Brown, Heather M.; Marin-Flores, Oscar G.; Bays, J. Timothy; Karim, Ayman M.*; Wang, Yong*
来源:Catalysis Today, 2016, 269: 103-109.
DOI:10.1016/j.cattod.2015.10.034

摘要

Aqueous phase processing of biomass derived sugar alcohols is one of the promising routes to convert biomass into fuels and chemicals. Bifunctional catalysts are critical in the aqueous phase hydrodeoxygenation of sugar alcohol. Understanding the interaction between metal and acidic metal oxides as well as the hydrodeoxygenation pathways will help develop more efficient bifunctional catalysts. Here, tungstated zirconia supported palladium catalysts were prepared and further characterized using nitrogen sorption, X-ray diffraction, FT-IR analysis of adsorbed pyridine, CO chemisorption and diffuse reflectance UV-vis. Strong interaction between palladium and WO3 in addition to a synergetic effect of the acidic and metallic sites were found to promote the aqueous phase hydrodeoxygenation of ethylene glycol. H-D exchange experiments using C-13{H-1} NMR spectroscopy confirmed that the aqueous phase hydrodeoxygenation follows a dehydration-hydrogenation pathway. The hydrogenation of the dehydration products shifts the dehydration-hydration equilibrium toward the dehydration pathway and leads to highly selective C-O cleavage.