Abstract

The main product of the conversion of ethanol to acetone on a ZnO-CaO catalyst is acetone, the yield of which strongly depends on the composition of the reaction environment. When oxygen is present, the yield of products of destructive and complete oxidation increases greatly. In contrast, when water vapor is present, both the selectivity and conversion of ethanol increase. Therefore, the conversion of ethanol is the limiting step in the overall process, which determines the selectivity of the conversion of ethanol to acetone. In this regard, it appeared suitable to investigate the effect of introducing water to the contact zone. As experiments indicated, the addition of water caused a significant effect on the conversion, selectivity, and acetone yield on the ZnO-CaO catalyst. As the partial pressure of water vapor increases, the conversion of ethanol and the acetone yield increase, while the yield of carbon dioxide decreases. The decrease in carbon dioxide is associated not only with the inhibition of the conversion of ethanol to CO2. In this study, the adsorption of water vapor and ammonia on the surface of the ZnO-CaO catalyst was examined by infrared spectroscopy method. It has been shown that water vapor at low temperatures is adsorbed on the catalyst surface in the molecular form, while at higher temperatures it is adsorbed in the dissociative form. Co-transformation reactions of ethanol with acetic acid, acetaldehyde with ethylene, and acetaldehyde with acetic acid have been studied. The obtained results indicated that acetone is formed mainly through the stage of complexation of acetaldehyde with ethylene. The isomerization reaction of 1-butene to 2-butene has been investigated. It was found that the yield of cis-2-butene in the absence of water vapor is higher, likely attributed to the molecular adsorption of water on Lewis centers. Based on these findings, a scheme for the vapor-phase conversion of ethanol into acetone on the studied catalysts was formulated.

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