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

Simon J. Freakley, Svenja Kochius, Jacqueline Marwijk, Caryn Fenner, Richard J. Lewis, Kai Baldenius, Sarel S. Marais, Diederik J. Opperman, Susan T. L. Harrison, Miguel Alcalde, Martha S. Smit () and Graham J. Hutchings ()
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Simon J. Freakley: Cardiff University, Main Building, Park Place
Svenja Kochius: University of the Free State
Jacqueline Marwijk: University of the Free State
Caryn Fenner: University of Cape Town, Private Bag, Rondebosch
Richard J. Lewis: Cardiff University, Main Building, Park Place
Kai Baldenius: BASF SE, RBW/OS - A 30
Sarel S. Marais: University of the Free State
Diederik J. Opperman: University of the Free State
Susan T. L. Harrison: University of Cape Town, Private Bag, Rondebosch
Miguel Alcalde: Institute of Catalysis, CSIC
Martha S. Smit: University of the Free State
Graham J. Hutchings: Cardiff University, Main Building, Park Place

Nature Communications, 2019, vol. 10, issue 1, 1-8

Abstract: 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.

Date: 2019
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DOI: 10.1038/s41467-019-12120-w

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