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Un grupo Cu4S de un solo agujero con N2O actividad de la reductasa: un modelo estructural y funcional para CuZ
Brittany J Johnson1, William E Antholine2, Sergey V Lindeman3
1Department of Chemistry, University of Illinois at Chicago , 845 West Taylor Street, Chicago, Illinois 60607, United States.
Journal of the American Chemical Society
|September 30, 2016
Resumen
Los investigadores han desarrollado un nuevo modelo de clúster de cobre y azufre que imita la enzima N2OR
Área de la Ciencia:
- Química bioorgánica
- Catálisis
- Ciencias del medio ambiente
Sus antecedentes:
- La desnitrificación bacteriana implica la reducción del óxido nitroso (N2O) a través de la enzima óxido nitroso reductasa (N2OR).
- El sitio catalítico de N2OR, conocido como CuZ*, contiene un grupo [Cu4 ((μ4-S) ] crucial para la reducción de N2O.
Objetivo del estudio:
- Sintetizar y caracterizar un nuevo grupo modelo de [Cu4(μ4-S) soportado por amidinato en su estado redox de un agujero.
- Establecer una serie redox completa de dos electrones de complejos modelo [Cu4(μ4-S] con estados de oxidación catalíticamente relevantes.
- Demostrar la imitación funcional del sitio activo CuZ* para la reducción de N2O.
Principales métodos:
- Síntesis de un grupo apoyado por amidinato [Cu4(μ4-S].
- Caracterización electroquímica del grupo en su estado redox de un agujero.
- Análisis espectroscópico para confirmar la estructura y las propiedades redox del cúmulo.
Principales resultados:
- El cúmulo de un agujero [Cu4(μ4-S] fue caracterizado a fondo.
- Este grupo, junto con sus socios redox, completa la serie redox de dos electrones de los complejos modelo [Cu4(μ4-S).
- El grupo de un agujero redujo con éxito el N2O a N2, formando el grupo de dos agujeros y completando un ciclo catalítico cerrado.
Conclusiones:
- El clúster sintetizado apoyado en amidinato [Cu4(μ4-S] es el mejor modelo estructural para el sitio activo de CuZ* hasta la fecha.
- Este complejo modelo funciona como una imitación efectiva de la enzima CuZ*, facilitando la reducción de N2O.
- El estudio proporciona información crucial sobre el mecanismo de reducción de N2O en la desnitrificación bacteriana.
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