Phenylacetylene Hydrogenation Coupled with Benzyl Alcohol Dehydrogenation over Cu/CeO2: A Consideration of Cu Oxidation State

Chiara Pischetola, Stephen M. Francis, Federico Grillo, Christopher J. Baddeley, Fernando Cardenas-Lizana

Research output: Contribution to journalArticlepeer-review

Abstract

We have examined the effect of copper oxidation state in the continuous gas phase coupled phenylacetylene hydrogenation (to styrene) with benzyl alcohol dehydrogenation (to benzaldehyde) over Cu/CeO2. Analysis by H2-TPR, XPS, XRD and STEM-EDX analyses demonstrates the generation of a range of Cu oxidation states (Cu0 (13-77%), Cu+ (13-74%), Cu2+ (0-55%)). The stepwise formation of styrene and ethylbenzene was promoted in the stand-alone phenylacetylene hydrogenation. An increase in Cu0/Cu+ (from H2-TPR and XPS) enhanced H2 chemisorption and styrene TOF, but with low hydrogen utilisation efficiency. The formation of benzaldehyde and toluene was promoted in the stand-alone dehydrogenation of benzyl alcohol, where benzaldehyde selectivity and TOF correlate with the concentration of Cu0. Full hydrogen utilisation, exclusive benzaldehyde/styrene formation and a (3-fold) greater styrene TOF (to attain 100% yield) was achieved in the coupled process, where hydrogenation/dehydrogenation activity correlates with Cu+/Cu0. This opens new directions for sustainable “hydrogen free” hydrogenations over non-noble Cu catalysts.
Original languageEnglish
JournalJournal of Catalysis
Early online date13 Nov 2020
DOIs
Publication statusE-pub ahead of print - 13 Nov 2020

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