A chemo-enzymatic oxidation cascade to activate C-H bonds with in situ generated H<sub>2</sub>O<sub>2</sub>.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 31519878.
- Also identified by DOI 10.1038/s41467-019-12120-w and PMC identifier 6744418.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
Abstract
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 ambient temperature and pressure to generate H<sub>2</sub>O<sub>2</sub> from H<sub>2</sub> and O<sub>2</sub> 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.