The potential of hydrodeoxygenation (HDO) for the upgrading of oxygenated feedstock is currently a hot research topic within the context of environmental chemistry. Specifically, the interest in biomass-derived pyrolysis oils (bio-oils) is justified by their potential to become a key bio-refinery stream, providing biofuels and/or platform chemicals. However, due to their intrinsically complex nature and the associated experimental hurdles, studies with actual bio-oils are lagging behind in comparison to model oxygenated components. Our work presents the continuous and stable HDO conversion of a raw black poplar bio-oil using PtPd/C and NiW/C catalysts with physically mixed HZSM-5 zeolite additives of different Si/Al ratios (15 and 140) pursuing enhanced yields of aromatic and (alkyl)phenolic components, which are valuable platform chemicals. After a fast initial deactivation period due to coke deposition, at TOS &gt; 4 h all the catalysts reach a pseudosteady activity state at which the carbon product yields are higher than in fresh catalyst conditions. The NiW/C+Z140 combination is the most efficient providing 47.3 wt% carbon products comprising 6.8 wt% phenolics and 15.5 wt% aromatics. This is a consequence of promoted synergies between the mildly acidic sites of the zeolite with the dehydrogenation activity of the metallic sites, hence favoring the acid-catalyzed cracking reaction of bio-oil oxygenates, while simultaneously limiting gas and coke formation reactions. Two different coke species are formed in the HDO process, namely thermal lignin (TL) and catalytic coke (CK). The development of the latter is enhanced by the PtPd/C catalyst and its combinations, particularly when mixed with a high-acidity Z15 zeolite, which boosts coke condensation reactions.

Stable production of platform chemicals from the continuous hydrodeoxygenation of a raw bio-oil using enhanced carbon-based catalysts

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

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