An immobilized and highly stabilized self-sufficientmonooxygenase as biocatalyst for oxidative biotransformations

Background: the requirement for expensive cofactors that must be efficiently recycled is one of the major factors hindering the wide implementation of industrial biocatalytic oxidation processes. In this research, a sustainable approach based on immobilized self-sufficient Baeyer-Villiger monooxygen...

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Detalles Bibliográficos
Autores: Valencia, Daniela|||0000-0002-5444-0509, Guillén, Marina|||0000-0002-9740-9966, Fürst, Maximilian JLJ, López Santín, Josep|||0000-0002-6039-8044, Álvaro, Gregorio|||0000-0002-2924-8902
Tipo de recurso: artículo
Fecha de publicación:2018
País:España
Institución:Universitat Autònoma de Barcelona
Repositorio:Dipòsit Digital de Documents de la UAB
Idioma:inglés
OAI Identifier:oai:ddd.uab.cat:196152
Acceso en línea:https://ddd.uab.cat/record/196152
https://dx.doi.org/urn:doi:10.1002/jctb.5450
Access Level:acceso abierto
Palabra clave:Cyclohexanone monooxygenase (CHMO)
Phosphite dehydrogenase (PTDH)
Multi-enzymatic reactions
Biocatalyst immobilization
Biocatalyst reutilization
Cofactor recycling
Descripción
Sumario:Background: the requirement for expensive cofactors that must be efficiently recycled is one of the major factors hindering the wide implementation of industrial biocatalytic oxidation processes. In this research, a sustainable approach based on immobilized self-sufficient Baeyer-Villiger monooxygenases is discussed. - Results: a bifunctional biocatalyst composed of an NADPH-dependent cyclohexanone monooxygenase (CHMO) fused to an NADP+-accepting phosphite dehydrogenase (PTDH) catalyzes ϵ-caprolactone synthesis from cyclohexanone, using phosphite as a cheap sacrificial substrate for cofactor regeneration. Several immobilized derivatives of the fused enzyme have been prepared with high immobilization yield (97%); the one obtained by affinity adsorption on Co-IDA (Co: cobalt chelated; IDA: iminodiacetic acid) support has shown to be highly stable affording average yields of 80% after 18 reaction cycles. - Conclusions -the immobilized self-sufficient monooxygenase has demonstrated to be able to perform Baeyer-Villiger oxidation with efficient cofactor recovery and biocatalyst recycling. The proposed biocatalytic process offers access to valuable molecules with high atom economy and limited waste generation.