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Protein Film Infrared Electrochemistry Demonstrated for Study of H2 Oxidation by a [NiFe] Hydrogenase
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Maduración de [FeFe]-hidrogenasa: Síntesis catalizada por hidrógeno de monóxido de carbono catalizada por hidrógeno
Eric M Shepard1, Benjamin R Duffus, Simon J George
1Department of Chemistry & Biochemistry and Astrobiology Biogeocatalysis Research Center, Montana State University, Bozeman, Montana 59717, USA.
Journal of the American Chemical Society
|June 23, 2010
Resumen
La enzima HydG sintetiza el monóxido de carbono (CO) de la tirosina, un paso crucial en la maduración de la [FeFe]-hidrogenasa. Esta es la primera demostración de la producción enzimática de CO en la biosíntesis de la hidrogenasa.
Área de la Ciencia:
- La bioquímica es la bioquímica.
- Enzimología Enzimología.
- Química organometálica Química orgánica de los metales.
Sus antecedentes:
- El sitio activo de la [FeFe]-hidrogenasa contiene un grupo H organometálico.
- Su biosíntesis requiere proteínas accesorias: HydE, HydG (enzimas radicales AdoMet) y HydF (GTPasa).
- El monóxido de carbono (CO) es un ligando común en los sitios activos de la hidrogenasa (sólo [FeFe], [NiFe], [Fe]).
Objetivo del estudio:
- Para investigar el papel de HydG en la biosíntesis del sitio activo de la hidrogenasa.
- Para determinar si el HydG cataliza la síntesis del monóxido de carbono (CO).
- Para identificar el sustrato para la producción de CO por HydG.
Principales métodos:
- Utilizó la desoxihemoglobina como un reportero para detectar la producción de CO.
- Se monitoreó la formación de carboxihemoglobina (HbCO) a través de la espectroscopia visible.
- Empleado (13) Espectroscopia infrarroja de C-tirosina y de la transformada de Fourier (FTIR) para confirmar el origen del CO.
Principales resultados:
- Se demostró que el HydG cataliza la síntesis de CO.
- Confirmado la tirosina como el sustrato para la producción de CO por HydG.
- Proporcionó la primera evidencia de la síntesis enzimática de CO durante la maduración de la hidrogenasa.
Conclusiones:
- HydG es responsable de la síntesis enzimática de CO de la tirosina.
- Este hallazgo aclara un paso clave en la compleja vía de maduración de la [FeFe]-hidrogenasa.
- Establece una nueva vía enzimática para la producción de CO relevante para la función de la hidrogenasa.
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