Cascading g-C3N4 and Peroxygenases for Selective Oxyfunctionalization Reactions

[EN] 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 HO can be addressed via in situ generation of...

Descripción completa

Detalles Bibliográficos
Autores: Van-Schie, Morten, Zhang, Wuyuan, Tieves, Florian, Choi, D.S., Park, Chan Beum, Burek, B.O., Bloh, Jonathan Z., Arends, I.W.C.E., Paul, Caroline E., Alcalde Galeote, Miguel, Hollmann, Frank
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2019
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/214468
Acceso en línea:http://hdl.handle.net/10261/214468
Access Level:acceso abierto
Palabra clave:Cascade reactions
Enzyme catalysis
Oxidation
Oxyfunctionalization
Photocatalysis
Descripción
Sumario:[EN] 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 HO can be addressed via in situ generation of HO. Here we report that simple graphitic carbon nitride (g-CN) 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.