Abstract
We study the selective catalytic oxidation of ethanol with air as a sustainable alternative route to acetaldehyde. The reaction is catalysed by molybdenum oxide supported on titania, in a flow reactor under ambient pressure. High selectivity to acetaldehyde (70%–89%, depending on the Mo loading) is obtained at 150 °C. Subsequently, we investigate the structure/performance relationship for various molybdenum oxide species using a combination of techniques including diffuse reflectance UV-visible, infrared, X-ray photoelectron spectroscopies, X-ray diffraction and temperature programmed reduction. As their surface density increases, the monomeric molybdenum oxide species undergo two-dimensional and three-dimensional oligomerisation. This results in polymolybdates and molybdenum oxide crystallites. Importantly, the ethanol oxidation rate depends not only on the overall molybdenum loading and dispersion, but also on the type of molybdenum oxide species prevalent at each surface density and on the domain size. As the molybdenum oxide oligomerisation increases, electron delocalisation becomes easier. This lowers the absorption edge energy and increases the reaction rate.
Highlights
While much research effort in industry and academia is directed towards sustainable chemicals production and biomass utilisation, petroleum-based processes still account for over 90% of carbon-containing chemicals.[1]
We study the selective catalytic oxidation of ethanol with air as a sustainable alternative route to acetaldehyde
We have studied titania-supported molybdenum oxide catalysts for the selective oxidation of ethanol to acetaldehyde
Summary
While much research effort in industry and academia is directed towards sustainable chemicals production and biomass utilisation, petroleum-based processes still account for over 90% of carbon-containing chemicals.[1] Most of these processes are highly efficient, reaping the benefits of many decades of optimisation and investment This means that if we really plan on introducing alternative routes to bulk chemicals starting from renewable resources, these must be simple and straightforward. The air oxidation (autooxidation) of ethanol to acetaldehyde [Eq (2)] could be a viable alternative, provided that a suitable catalyst is found
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