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Selective Ammoximation of Ketones via In Situ H2O2 Synthesis

Lewis, Richard J., Ueura, Kenji, Liu, Xi, Fukuta, Yukimasa, Qin, Tian, Davies, Thomas, Morgan, David J. ORCID: https://orcid.org/0000-0002-6571-5731, Stenner, Alex, Singleton, James, Edwards, Jennifer K. ORCID: https://orcid.org/0000-0003-4089-2827, Freakley, Simon J., Kiely, Christopher J. ORCID: https://orcid.org/0000-0001-5412-0970, Chen, Liwei, Yamamoto, Yasushi and Hutchings, Graham J. ORCID: https://orcid.org/0000-0001-8885-1560 2023. Selective Ammoximation of Ketones via In Situ H2O2 Synthesis. ACS Catalysis 13 , pp. 1934-1945. 10.1021/acscatal.2c05799

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Abstract

The ammoximation of ketones to the corresponding oxime via the in situ production of H2O2 offers a viable alternative to the current means of industrial-scale production, in particular for the synthesis of cyclohexanone oxime, a key precursor to Nylon-6. Herein, we demonstrate that using a bifunctional catalyst, consisting of Pd-based bimetallic nanoparticles immobilized onto a TS-1 carrier, it is possible to bridge the considerable condition gap that exists between the two key distinct reaction pathways that constitute an in-situ approach (i.e., the direct synthesis of H2O2 and ketone ammoximation). The formation of PdAu nanoalloys is found to be crucial in achieving high reactivity and in promoting catalytic stability, with the optimal formulation significantly outperforming both alternative Pd-based materials and the monometallic Pd analogue.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Cardiff Catalysis Institute (CCI)
Publisher: American Chemical Society
ISSN: 2155-5435
Funders: Max Planck Centre for Fundamental Heterogeneous Catalysis (FUNCAT)
Date of First Compliant Deposit: 27 January 2023
Date of Acceptance: 6 January 2023
Last Modified: 11 Oct 2023 20:38
URI: https://orca.cardiff.ac.uk/id/eprint/156317

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