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

Simon J. Freakley, Svenja Kochius, Jacqueline van Marwijk, Caryn Fenner, Richard J. Lewis, Kai Baldenius, Sarel S. Marais, Diederik J. Opperman, Susan T.L. Harrison, Miguel Alcalde, Martha S. Smit, Graham J. Hutchings

Research output: Contribution to journalArticle

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.

Original languageEnglish
Article number4178
Pages (from-to)1-8
Number of pages8
JournalNature Communications
Volume10
Issue number1
DOIs
Publication statusPublished - 13 Sep 2019

ASJC Scopus subject areas

  • Chemistry(all)
  • Biochemistry, Genetics and Molecular Biology(all)
  • Physics and Astronomy(all)

Cite this

Freakley, S. J., Kochius, S., van Marwijk, J., Fenner, C., Lewis, R. J., Baldenius, K., ... Hutchings, G. J. (2019). A chemo-enzymatic oxidation cascade to activate C-H bonds with in situ generated H2O2. Nature Communications, 10(1), 1-8. [4178]. https://doi.org/10.1038/s41467-019-12120-w

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.; Hutchings, Graham J.

In: Nature Communications, Vol. 10, No. 1, 4178, 13.09.2019, p. 1-8.

Research output: Contribution to journalArticle

Freakley, SJ, Kochius, S, van Marwijk, J, Fenner, C, Lewis, RJ, Baldenius, K, Marais, SS, Opperman, DJ, Harrison, STL, Alcalde, M, Smit, MS & Hutchings, GJ 2019, 'A chemo-enzymatic oxidation cascade to activate C-H bonds with in situ generated H2O2', Nature Communications, vol. 10, no. 1, 4178, pp. 1-8. https://doi.org/10.1038/s41467-019-12120-w
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. ; Hutchings, Graham J. / A chemo-enzymatic oxidation cascade to activate C-H bonds with in situ generated H2O2. In: Nature Communications. 2019 ; Vol. 10, No. 1. pp. 1-8.
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