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Phenylacetylene hydrogenation coupled with benzyl alcohol dehydrogenation over Cu/CeO2 : a consideration of Cu oxidation state
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dc.contributor.author | Pischetola, Chiara | |
dc.contributor.author | Francis, Stephen M. | |
dc.contributor.author | Grillo, Federico | |
dc.contributor.author | Baddeley, Christopher J. | |
dc.contributor.author | Cárdenas-Lizana, Fernando | |
dc.date.accessioned | 2021-11-13T00:45:22Z | |
dc.date.available | 2021-11-13T00:45:22Z | |
dc.date.issued | 2020-11-13 | |
dc.identifier | 271287912 | |
dc.identifier | e5b7b01d-594f-49bb-93be-2f5a5c76e7d7 | |
dc.identifier | 85097054867 | |
dc.identifier | 000624652500015 | |
dc.identifier.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 | en |
dc.identifier.issn | 0021-9517 | |
dc.identifier.other | RIS: urn:205A669E4B138000EF1066859CFA2B41 | |
dc.identifier.other | ORCID: /0000-0001-9961-1212/work/83889417 | |
dc.identifier.other | ORCID: /0000-0001-9750-6494/work/83889455 | |
dc.identifier.uri | https://hdl.handle.net/10023/24335 | |
dc.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]. | en |
dc.description.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. | |
dc.format.extent | 3292276 | |
dc.language.iso | eng | |
dc.relation.ispartof | Journal of Catalysis | en |
dc.subject | Coupling process | en |
dc.subject | phenylacetylene hydrogenation | en |
dc.subject | benzylalcoholdehydrogenation | en |
dc.subject | Copper oxidation sate | en |
dc.subject | Cu/CeO | en |
dc.subject | QD Chemistry | en |
dc.subject | DAS | en |
dc.subject.lcc | QD | en |
dc.title | Phenylacetylene hydrogenation coupled with benzyl alcohol dehydrogenation over Cu/CeO2 : a consideration of Cu oxidation state | en |
dc.type | Journal article | en |
dc.contributor.institution | University of St Andrews. School of Chemistry | en |
dc.contributor.institution | University of St Andrews. EaSTCHEM | en |
dc.identifier.doi | 10.1016/j.jcat.2020.11.002 | |
dc.description.status | Peer reviewed | en |
dc.date.embargoedUntil | 2021-11-13 |
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