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Phenylacetylene hydrogenation coupled with benzyl alcohol dehydrogenation over Cu/CeO2 : a consideration of Cu oxidation state

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Pischetola_2020_JC_Phenylacetylene_AAM.pdf (3.139Mb)
Date
13/11/2020
Author
Pischetola, Chiara
Francis, Stephen M.
Grillo, Federico
Baddeley, Christopher J.
Cárdenas-Lizana, Fernando
Keywords
Coupling process
phenylacetylene hydrogenation
benzylalcoholdehydrogenation
Copper oxidation sate
Cu/CeO
QD Chemistry
DAS
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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.
Citation
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
Publication
Journal of Catalysis
Status
Peer reviewed
DOI
https://doi.org/10.1016/j.jcat.2020.11.002
ISSN
0021-9517
Type
Journal article
Rights
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
Description
We 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].
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  • University of St Andrews Research
URI
http://hdl.handle.net/10023/24335

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