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Tunable copper-hydrotalcite derived mixed oxides for sustainable ethanol condensation to n-butanol in liquid phase

Benito, Patricia, Vaccari, Angelo, Antonetti, Claudia, Licursi, Domenico, Schiarioli, Nicola, Rodriguez-Castellón, Enrique, Raspolli Galletti, Anna Maria
Journal of cleaner production 2019 v.209 pp. 1614-1623
acetone, aluminum, batch systems, biofuels, butanol, carbon, catalysts, catalytic activity, copper, ethanol, feedstocks, liquids, magnesium, oxides
Improvement of processes starting from renewable feedstocks to produce chemicals and biofuels up to now derived from fossil carbon feedstocks is paramount to creating environmentally sustainable industrial processes. Guerbet condensation of ethanol to give n-butanol represents a turning point not only respect to the traditional petrochemical “oxo” process, but also to the bio-chemical path (Acetone Butanol Ethanol “ABE” process). In this work, different Cu/Mg/Al hydrotalcite-derived mixed oxides catalysts, with Cu atomic content in the range 7.6–1.0%, were synthetised, characterized, and tested for the Guerbet reaction. The adopted catalysts are easy to produce, and based on available, cheap and non-toxic metals. Tailoring Cu-content in hydrotalcite-derived Cu/Mg/Al mixed oxides allowed us to selectively address this reaction towards n-butanol formation, highlighting how a low Cu-content favours the condensation to n-butanol and higher alcohols, in particular n-hexanol, decreasing the ester formation. The Guerbet selective co-production of [n-butanol + n-hexanol] is economically even more attractive than that of the sole n-butanol, being both saleable products. Good catalytic performances to n-butanol and n-hexanol were achieved, in a batch process carried out under subcritical conditions. These catalysts have required a simple procedure of recovery, showing good recyclability, in term of catalytic performances to give the target products, thus opening the way to applicative perspectives.