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El mecanismo semirreducido para la reducción de óxido nítrico por complejos de diironio no hemo: modelado de las

Corey J White¹, Amy L Speelman¹, Claudia Kupper²

¹Department of Chemistry, The University of Michigan , Ann Arbor, Michigan 48109-1055, United States.

Journal of the American Chemical Society

|January 20, 2018

Resumen

Las reductasas de óxido nítrico de flavodiero (FNOR) reducen el óxido nítrico (NO) a N₂O. Un complejo modelo demuestra que esta reducción se produce de manera eficiente a través de un mecanismo semirreducido, que ofrece información sobre la resistencia bacteriana y la catálisis sintética.

Área de la Ciencia:

Química bioorgánica
Mecanismos de las enzimas
Catálisis

Sus antecedentes:

Las reductasas de óxido nítrico de flavodiero (FNOR) son cruciales para las bacterias patógenas, permitiendo la supervivencia contra el estrés nitrosante mediante la reducción del óxido nítrico (NO) a N₂O.
La comprensión del mecanismo de reducción de NO por FNOR es vital para el desarrollo de estrategias contra las infecciones bacterianas y para el diseño de nuevos catalizadores sintéticos.

Objetivo del estudio:

Para caracterizar espectroscópicamente y estudiar la reactividad de un complejo modelo de diiron dinitrosyl, [Fe₂(BPMP) ((OPr) ((NO) ₂] ((OTf) ₂, imitando el sitio activo FNOR.
Para aclarar el mecanismo y la eficiencia de la reducción de óxido nítrico (NO) a óxido nitroso (N₂O) por este complejo modelo.

Principales métodos:

Espectroscopia UV-vis
Voltametría cíclica
Espectro-electroquímica
Estudios de etiquetado por isótopos

Principales resultados:

El complejo modelo reduce cuantitativamente el NO a N₂O utilizando un único equivalente reductor a través de un mecanismo semirreducido con una constante de alta velocidad (k > 10² s^-1).
El etiquetado de isótopos confirmó un mecanismo de acoplamiento N-N intramolecular, consistente con una rápida reducción y una baja barrera de formación de enlaces N-N.
La reacción continúa eficientemente a -80 °C, lo que permite la observación del intermedio de valor mixto; las temperaturas más altas conducen a la descomposición del producto.

Conclusiones:

El mecanismo semirreducido es una vía altamente eficiente para la reducción de NO a N₂O en FNOR y catalizadores sintéticos.
Se obtuvieron conocimientos mecanicistas detallados sobre la reducción de NO por el complejo [Fe₂(BPMP) ((OPr) ((NO) ₂]²⁺, validando su papel como modelo de sitio activo FNOR.

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