To counteract the effects of global warming, research into renewable, carbon neutral fuels is required. H2 is the ideal clean burning fuel, releasing environmentally benign water as the only combustion product. The motivation of this research is to produce H2 fuel from renewable feedstocks such as biomass (eg, bio-alcohols) in an inexpensive and facile manner. This led us to explore the fundamental chemistry of uncalcined, single site, Mo-dioxo catalysts towards alcohols. The catalyst was prepared by grafting a known organometallic Mo-dioxo catalyst on activated carbon, and was fully characterized by X-ray adsorption, powder-X-ray diffraction, and surface chemisorption techniques. This catalyst shows unprecedented reactivity towards both methanol and ethanol at ambient pressure, releasing 1 equivalent of H2 (up to 100% yields) with concomitant generation of oligomeric aldehydes between 40 and 90 °C. The catalyst is fully recyclable over 20 additions of fresh alcohol, and shows no deactivation in up to 90 % water. In contrast to current state of the art catalysts for this transformation, the stability and high activity of this catalyst permit its use in direct methanol fuel cells. These results provide a new carbon neutral process for the production of renewable H2 fuel from biomass.

Hydrogen and formaldehyde generation from bio-derived alcohols using supported molybdenum-oxo catalysts

253rd National Meeting (2017)

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