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Controlling product selectivity with nanoparticle composition in tandem chemo-biocatalytic styrene oxidation

Wilbers, Derik, Brehm, Joseph, Lewis, Richard, Van Marwijk, Jacqueline, Davies, Thomas, Morgan, David John, Opperman, Diederik J., Smit, Martha Sophia, Alcalde, Miguel, Kotsiopoulos, Athanasios, Harrison, Susan T. L., Hutchings, Graham and Freakley, Simon 2021. Controlling product selectivity with nanoparticle composition in tandem chemo-biocatalytic styrene oxidation. Green Chemistry 23 (11) , pp. 4170-4180. 10.1039/D0GC04320F

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Abstract

The combination of heterogeneous catalysis and biocatalysis into one-pot reaction cascades is a potential approach to integrate enzymatic transformations into existing chemical infrastructure. Peroxygenases, which can achieve clean C-H activation, are ideal candidates for incorporation into such tandem systems; however a constant supply of low-level hydrogen peroxide (H2O2) is required. The use of such enzymes at industrial scale will likely necessitate the in situ generation of the oxidant from cheap and widely available reactants. We show that combing heterogeneous catalysts (AuxPdy/TiO2) to produce H2O2 in situ from H2 and air, in the presence of an evolved unspecific peroxygenase from Agrocybe aegerita (PaDa-I variant) yields a highly active cascade process capable of oxidizing alkyl and alkenyl substrates under mild conditions. When alkenes such as styrene are subjected to this tandem oxidation process, divergent reaction pathways are observed due to the competing hydrogenation of the alkene by palladium rich nanoparticles in the presence of H2. Each pathway presents opportunities for value added products. Product selectivity was highly sensitive to the rate of reduction compared to hydrogen peroxide delivery. Here we show that some control over product selectivity may be exerted by careful selection of nanoparticle composition.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Cardiff Catalysis Institute (CCI)
Additional Information: This article is licensed under a Creative Commons Attribution 3.0 Unported Licence
Publisher: Royal Society of Chemistry
ISSN: 1463-9262
Date of First Compliant Deposit: 11 May 2021
Date of Acceptance: 7 May 2021
Last Modified: 30 Jan 2022 11:56
URI: https://orca.cardiff.ac.uk/id/eprint/141220

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