Phenylacetylene hydrogenation coupled with benzyl alcohol dehydrogenation over Cu/CeO2 : a consideration of Cu oxidation state
MetadataShow full item record
Altmetrics Handle Statistics
Altmetrics DOI Statistics
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.
Pischetola , C , Francis , S M , Grillo , F , Baddeley , C J & Cárdenas-Lizana , F 2020 , ' Phenylacetylene hydrogenation coupled with benzyl alcohol dehydrogenation over Cu/CeO 2 : a consideration of Cu oxidation state ' , Journal of Catalysis , vol. In press . https://doi.org/10.1016/j.jcat.2020.11.002
Journal of Catalysis
Copyright © 2020 Elsevier Inc. All rights reserved. This work has been made available online in accordance with publisher policies or with permission. Permission for further reuse of this content should be sought from the publisher or the rights holder. This is the author created accepted manuscript following peer review and may differ slightly from the final published version. The final published version of this work is available at https://doi.org/10.1016/j.jcat.2020.11.002
DescriptionWe shall acknowledge the Engineering and Physical Sciences Research Council, University of Heriot-Watt, and CRITICAT Centre for Doctoral Training for financial support [Ph.D. studentship to Chiara Pischetola; Grant EP/L016419/1].
Items in the St Andrews Research Repository are protected by copyright, with all rights reserved, unless otherwise indicated.