Efficient bioelectrocatalytic NADH regeneration with a novel amino-functionalized viologen redox polymer

Oxidoreductase enzymes, used for a variety of applications including organic synthesis and pharmaceutical industry, require reduced nicotinamide adenine dinucleotide (NADH) as reducing equivalents. Methods for regenerating NAD+ to NADH are of significant interest due to the high cost and stoichiomet...

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Detalles Bibliográficos
Autores: Jayakumar, Kavita, Fera, Mihai-Cristian, Abad, José M., López de Lacey, Antonio, Pita, Marcos
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2025
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/397655
Acceso en línea:http://hdl.handle.net/10261/397655
https://api.elsevier.com/content/abstract/scopus_id/85210546689
Access Level:acceso embargado
Palabra clave:Bioelectrochemistry
Bioelectrosynthesis
Redox polymer
Viologen
Descripción
Sumario:Oxidoreductase enzymes, used for a variety of applications including organic synthesis and pharmaceutical industry, require reduced nicotinamide adenine dinucleotide (NADH) as reducing equivalents. Methods for regenerating NAD+ to NADH are of significant interest due to the high cost and stoichiometric amounts of cofactor required. Diaphorase/redox mediator systems have shown promise for this purpose, but suitable mediators are few due to the low redox potential required, necessary downstream processing and stability issues. A novel amino-functionalized viologen is presented in this work which, upon immobilization with diaphorase, yields bioactive NADH with high selectivity (99 %) and faradaic efficiency (99 %). This system was tested with NADH-dependent formate dehydrogenase, showing a 21-fold improvement in formate yield compared to an enzymatic negative control without NADH regeneration. The findings underscore the potential of this novel amino-functionalized viologen polymer to advance sustainable and efficient NADH regeneration at very low overpotential.