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

Author

Listed:
  • Simon J. Freakley

    (Cardiff University, Main Building, Park Place
    University of Bath)

  • Svenja Kochius

    (University of the Free State
    University of Cape Town, Private Bag, Rondebosch)

  • Jacqueline Marwijk

    (University of the Free State
    University of Cape Town, Private Bag, Rondebosch)

  • Caryn Fenner

    (University of Cape Town, Private Bag, Rondebosch
    University of Cape Town)

  • 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
    University of Cape Town, Private Bag, Rondebosch)

  • Diederik J. Opperman

    (University of the Free State
    University of Cape Town, Private Bag, Rondebosch)

  • Susan T. L. Harrison

    (University of Cape Town, Private Bag, Rondebosch
    University of Cape Town)

  • Miguel Alcalde

    (Institute of Catalysis, CSIC)

  • Martha S. Smit

    (University of the Free State
    University of Cape Town, Private Bag, Rondebosch)

  • Graham J. Hutchings

    (Cardiff University, Main Building, Park Place)

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.

Suggested Citation

  • 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. S, 2019. "A chemo-enzymatic oxidation cascade to activate C–H bonds with in situ generated H2O2," Nature Communications, Nature, vol. 10(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-12120-w
    DOI: 10.1038/s41467-019-12120-w
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