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A chemo-enzymatic oxidation cascade to activate C–H bonds with in situ generated H(2)O(2)
Continuous low-level supply or in situ generation of hydrogen peroxide (H(2)O(2)) 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 th...
Autores principales: | , , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2019
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6744418/ https://www.ncbi.nlm.nih.gov/pubmed/31519878 http://dx.doi.org/10.1038/s41467-019-12120-w |
Sumario: | Continuous low-level supply or in situ generation of hydrogen peroxide (H(2)O(2)) 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(2) or carbon have sufficient activity at ambient temperature and pressure to generate H(2)O(2) from H(2) and O(2) 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. |
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