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

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.

SUBMITTER: Freakley SJ 

PROVIDER: S-EPMC6744418 | biostudies-literature | 2019 Sep

REPOSITORIES: biostudies-literature

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A chemo-enzymatic oxidation cascade to activate C-H bonds with in situ generated H<sub>2</sub>O<sub>2</sub>.

Freakley Simon J SJ   Kochius Svenja S   van Marwijk Jacqueline J   Fenner Caryn C   Lewis Richard J RJ   Baldenius Kai K   Marais Sarel S SS   Opperman Diederik J DJ   Harrison Susan T L STL   Alcalde Miguel M   Smit Martha S MS   Hutchings Graham J GJ  

Nature communications 20190913 1

Continuous low-level supply or in situ generation of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) 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 TiO<sub>2</sub> or carbon have sufficient activity at  ...[more]

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