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A chemo-enzymatic oxidation cascade to activate C-H bonds with in situ generated H2O2

Freakley, Simon J., Kochius, Svenja, van Marwijk, Jacqueline, Fenner, Caryn, Lewis, Richard J., Baldenius, Kai, Marais, Sarel S., Opperman, Diederik J., Harrison, Susan T. L., Alcalde, Miguel, Smit, Martha S. and Hutchings, Graham J. 2019. A chemo-enzymatic oxidation cascade to activate C-H bonds with in situ generated H2O2. Nature Communications 10 (1) , 4178. 10.1038/s41467-019-12120-w

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Abstract

Continuous low-level supply or in situ generation of hydrogen peroxide (H2O2) is essential for the stability of unspecific peroxygenases, which are deemed ideal biocatalysts for the selective activation of C–H bonds. To envisage potential large scale applications of combined catalytic systems the reactions need to be simple, efficient and produce minimal by-products. We show that gold-palladium nanoparticles supported on TiO2 or carbon have sufficient activity at ambient temperature and pressure to generate H2O2 from H2 and O2 and supply the oxidant to the engineered unspecific heme-thiolate peroxygenase PaDa-I. This tandem catalyst combination facilitates efficient oxidation of a range of C-H bonds to hydroxylated products in one reaction vessel with only water as a by-product under conditions that could be easily scaled. https://doi.org/10.1038/s41467-019-12120-w OPEN 1

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Cardiff Catalysis Institute (CCI)
Publisher: Nature Research
ISSN: 2041-1723
Funders: MAXNET Energy Consortium
Date of First Compliant Deposit: 1 October 2019
Date of Acceptance: 16 August 2019
Last Modified: 02 Oct 2019 10:15
URI: http://orca-mwe.cf.ac.uk/id/eprint/125812

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