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Reducción del dióxido de carbono por una deshidrogenasa de formato que contiene molibdeno: un estudio cinético y

Luisa B Maia¹, Luis Fonseca¹, Isabel Moura¹

¹UCIBIO, REQUIMTE, Departamento de Química, Faculdade de Ciências e Tecnologia, Universidade Nova de Lisboa , 2829-516 Caparica, Portugal.

Journal of the American Chemical Society

|June 28, 2016

Resumen

Desulfovibrio desulfuricans formate dehydrogenase (Dd FDH) puede activar y convertir eficientemente el dióxido de carbono en combustibles. Esta enzima

Área de la Ciencia:

Biocatálisis y mecanismos enzimáticos
Química ambiental y sostenibilidad

Sus antecedentes:

La acumulación de dióxido de carbono (CO2) plantea riesgos ecológicos, sin embargo, su bajo costo y abundancia lo convierten en una materia prima valiosa.
La estabilidad de la molécula de CO2 presenta desafíos para su activación y utilización química.
Las estrategias catalíticas inspiradas en la naturaleza son fundamentales para el desarrollo de biocatalizadores eficientes para la conversión de CO2.

Objetivo del estudio:

Caracterizar cinética y mecanicamente la actividad de reducción de dióxido de carbono de Desulfovibrio desulfuricans formate dehydrogenase (Dd FDH).
Investigar el mecanismo de activación y la reversibilidad catalítica de Dd FDH.
Proponer un nuevo mecanismo de reacción para la oxidación del formato y la reducción del CO2.

Principales métodos:

Caracterización cinética de las reacciones catalizadas por Dd FDH.
Estudios mecánicos relacionados con la activación e inhibición de enzimas.
Desarrollo de un modelo cinético para el comportamiento de las enzimas histéricas.
Análisis espectroscópico de los centros de molibdeno.

Principales resultados:

Dd FDH requiere un proceso de activación dependiente de la reducción, exhibiendo histeresis.
El Dd FDH activado cataliza eficientemente tanto la oxidación del formato (kcat = 543 s-1, Km = 57,1 μM) como la reducción del CO2 (kcat = 46,6 s-1, Km = 15,7 μM).
Ambas reacciones son reversibles e inhibidas por el cianuro.
Se propone un nuevo mecanismo que implica la transferencia de hidruro y las interacciones molibdeno-azufre.

Conclusiones:

Dd FDH es un biocatalizador prometedor para la utilización reversible del CO2.
La comprensión de los mecanismos de activación y reacción de las enzimas puede guiar el diseño de nuevos catalizadores de conversión de CO2.
El mecanismo propuesto pone de relieve el papel del grupo sulfo de molibdeno en la transferencia de hidritos.

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