Cascading g-C₃N₄ and Peroxygenases for Selective Oxyfunctionalization Reactions

Cascading g-C₃N₄ and Peroxygenases for Selective Oxyfunctionalization Reactions

van Schie, M.M.C.H. (TU Delft BT/Biocatalysis)
Zhang, W. (TU Delft BT/Biocatalysis)
Tieves, F. (TU Delft BT/Biocatalysis)
Choi, Da Som (Korea Advanced Institute of Science and Technology)
Park, Chan Beum (Korea Advanced Institute of Science and Technology)
Burek, Bastien O. (DECHEMA Forschungsinstitut)
Bloh, Jonathan Z. (DECHEMA Forschungsinstitut)
Arends, I.W.C.E. (Universiteit Utrecht)
Paul, C.E. (TU Delft BT/Biocatalysis)
Alcalde, Miguel (Institute of Catalysis, CSIC, Madrid)
Hollmann, F. (TU Delft BT/Biocatalysis)

2019

Peroxygenases are very interesting catalysts for specific oxyfunctionalization chemistry. Instead of relying on complicated electron transport chains, they rely on simple hydrogen peroxide as the stoichiometric oxidant. Their poor robustness against H₂O₂ can be addressed via in situ generation of H₂O₂. Here we report that simple graphitic carbon nitride (g-C₃N₄) is a promising photocatalyst to drive peroxygenase-catalyzed hydroxylation reactions. The system has been characterized by outlining not only its scope but also its current limitations. In particular, spatial separation of the photocatalyst from the enzyme is shown as a solution to circumvent the undesired inactivation of the biocatalyst. Overall, very promising turnover numbers of the biocatalyst of more than 60.000 have been achieved.

cascade reactions
enzyme catalysis
oxidation
oxyfunctionalization
photocatalysis

http://resolver.tudelft.nl/uuid:43e3eb49-af3b-4287-aa2b-5497e0d7f00a

https://doi.org/10.1021/acscatal.9b01341

2155-5435

ACS Catalysis, 9 (8), 7409-7417

Institutional Repository

journal article

© 2019 M.M.C.H. van Schie, W. Zhang, F. Tieves, Da Som Choi, Chan Beum Park, Bastien O. Burek, Jonathan Z. Bloh, I.W.C.E. Arends, C.E. Paul, Miguel Alcalde, F. Hollmann