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Cyclohexanone ammoximation via in situ H2O2 production using TS-1 supported catalysts

Lewis, Richard J., Ueura, Kenji, Fukuta, Yukimasa, Davies, Thomas E., Morgan, David J. ORCID: https://orcid.org/0000-0002-6571-5731, Paris, Charlie, Singleton, James, Edwards, Jennifer. K. ORCID: https://orcid.org/0000-0003-4089-2827, Freakley, Simon J., Yamamoto, Yasushi and Hutchings, Graham J. ORCID: https://orcid.org/0000-0001-8885-1560 2022. Cyclohexanone ammoximation via in situ H2O2 production using TS-1 supported catalysts. Green Chemistry 24 , pp. 9496-9507. 10.1039/D2GC02689A

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Abstract

The ammoximation of cyclohexanone to the corresponding oxime via in situ H2O2 formation offers an attractive alternative to the current industrial means of production, overcoming the significant economic and environmental concerns associated with the manufacture of a key reagent, H2O2. Herein we demonstrate the efficacy of a composite catalyst, consisting of precious metal nanoparticles supported on a commercial TS-1, towards the in situ synthesis of cyclohexanone oxime, bridging the wide condition gap that exists between the two distinct reaction pathways: H2O2 direct synthesis and cyclohexanone ammoximation. In particular, the alloying of Au with Pd and the introduction of low concentrations of Pt into AuPd nanoalloys are found to be key in promoting high catalytic performance. The improved catalytic activity of optimal catalysts is found to result from a combination of a disruption of contiguous Pd ensembles and the modification of Pd oxidation states, which in turn dictate catalytic activity towards the production and subsequent degradation of H2O2.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Cardiff Catalysis Institute (CCI)
Publisher: Royal Society of Chemistry
ISSN: 1463-9262
Funders: EPSRC
Date of First Compliant Deposit: 13 October 2022
Date of Acceptance: 8 September 2022
Last Modified: 12 Jan 2023 13:55
URI: https://orca.cardiff.ac.uk/id/eprint/153359

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