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Formación y estructura electrónica de un sitio atípico Cu_A

Matthew O Ross, Oriana S Fisher, Marcos N Morgada^1,2

¹Instituto de Biología Molecular y Celular de Rosario (IBR, CONICET-UNR) , Ocampo y Esmeralda, 2000 Rosario , Argentina.

Journal of the American Chemical Society

|February 27, 2019

Resumen

La proteína PmoD de las bacterias oxidantes de metano forma un centro único de Cu_A. Este estudio revela su distinta estructura electrónica e inestabilidad, expandiendo la diversidad conocida de sitios Cu_A.

Área de la Ciencia:

La bioquímica
La biofísica
Microbiología

Sus antecedentes:

PmoD es una proteína de bacterias oxidantes de metano que contiene un centro de Cu_A.
Los sitios canónicos Cu_A exhiben firmas ópticas y espectroscópicas específicas.
El sitio Cu_A de PmoD muestra similitudes pero también diferencias desconcertantes en comparación con los sitios canónicos.

Objetivo del estudio:

Para caracterizar la formación, el decaimiento, la estructura electrónica y geométrica del sitio PmoD Cu_A.
Para comparar PmoD Cu_A con otros sitios conocidos de Cu_A.
Para entender las propiedades únicas de este centro bacteriano Cu_A.

Principales métodos:

Espectroscopia óptica de flujo detenido
Espectroscopias de resonancia paramagnética avanzadas (EPR, ENDOR, ESEEM y HYSCORE)
Espectroscopia de resonancia magnética nuclear (RMN)

Principales resultados:

El sitio PmoD Cu_A se forma rápidamente (segundos) y se descompone lentamente (horas) a dos sitios Cu²⁺ mononucleares.
Se observó un intermedio de corta duración con λ_max 360 nm durante la formación.
PmoD Cu_A exhibe un estado base σ_u* puro, a diferencia de otras proteínas Cu_A.
La coordinación del ligando involucra dos histidinas y dos cisteínas de manera simétrica.

Conclusiones:

El sitio PmoD Cu_A es inestable y distinto de los sitios canónicos Cu_A.
Su estructura electrónica única y su entorno de ligandos amplían la diversidad conocida de centros Cu_A.
Esta investigación mejora la comprensión de las interacciones cobre-proteína en las bacterias oxidantes de metano.

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