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

Authors :
Ministerio de Economía y Competitividad (España)
University of Bath
Claude Leon Foundation
Opperman, Diederik J. [0000-0002-2737-8797]
Harrison, Susan T.L. [0000-0002-2268-3506]
Alcalde Galeote, Miguel [0000-0001-6780-7616]
Smit, Martha S. [0000-0002-1295-6507]
Hutchings, Graham J. [0000-0001-8885-1560]
Freakley, Simon J.
Kochius, Svenja
Marwijk, Jacqueline van
Fenner, Caryn
Lewis, Richard J.
Baldenius, Kai
Marais, Sarel S.
Opperman, Diederik J.
Harrison, Susan T.L.
Alcalde Galeote, Miguel
Smit, Martha S.
Hutchings, Graham J.
Ministerio de Economía y Competitividad (España)
University of Bath
Claude Leon Foundation
Opperman, Diederik J. [0000-0002-2737-8797]
Harrison, Susan T.L. [0000-0002-2268-3506]
Alcalde Galeote, Miguel [0000-0001-6780-7616]
Smit, Martha S. [0000-0002-1295-6507]
Hutchings, Graham J. [0000-0001-8885-1560]
Freakley, Simon J.
Kochius, Svenja
Marwijk, Jacqueline van
Fenner, Caryn
Lewis, Richard J.
Baldenius, Kai
Marais, Sarel S.
Opperman, Diederik J.
Harrison, Susan T.L.
Alcalde Galeote, Miguel
Smit, Martha S.
Hutchings, Graham J.
Publication Year :
2019

Abstract

[EN] 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.

Details

Database :
OAIster
Publication Type :
Electronic Resource
Accession number :
edsoai.on1286542147
Document Type :
Electronic Resource