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Un complejo no hemo de alto espín que genera espontáneamente N2O
Alex M Confer1, Alison C McQuilken1, Hirotoshi Matsumura2
1Department of Chemistry, Johns Hopkins University , Baltimore, Maryland 21218, United States.
Journal of the American Chemical Society
|July 28, 2017
Resumen
Los investigadores sintetizaron un complejo no hemo de hierro-nitrosilo (FeNO8) que genera óxido nitroso (N2O). Este descubrimiento ofrece nuevos conocimientos sobre los mecanismos de las enzimas reductasas de óxido nítrico.
Área de la Ciencia:
- Química bioorgánica
- Química organometálica
- Mecanismos de las enzimas
Sus antecedentes:
- Los complejos de hierro-nitrosilo no hemo son cruciales en los sistemas biológicos.
- La comprensión de las reductasas de óxido nítrico (NOR) es vital para el ciclo del nitrógeno y la bioenergética.
- Los estudios anteriores se han centrado en los NOR que contienen hemo, dejando los sistemas no hemo menos explorados.
Objetivo del estudio:
- Para sintetizar y caracterizar un nuevo complejo no hemo.
- Investigar la reactividad y la generación de N2O de este complejo.
- Para aclarar los mecanismos potenciales relevantes para las reductasas de óxido nítrico no hemo.
Principales métodos:
- Reducción de un electrón de un complejo precursor de hierro-nitrosilo ([Fe(NO) -[N3PyS) ]BF4).
- Síntesis del complejo objetivo mediante la adición de ácido de Piloty (un donante de HNO) a un precursor de FeII.
- Caracterización de las especies no heme resultantes.
Principales resultados:
- Se produjo con éxito un complejo no hemo {FeNO}8, [Fe(NO) ((N3PyS).
- Este complejo es un raro ejemplo de una especie de alto espín (S = 1) {FeNO} .
- Es el primer complejo no hemo mononuclear reportado capaz de generar N2O.
Conclusiones:
- El estudio presenta un nuevo complejo no hemo con una reactividad única.
- La generación de N2O a partir de este complejo proporciona información sobre los mecanismos NOR.
- Este trabajo abre nuevas vías para el estudio de las enzimas que no contienen hierro hemo involucradas en el metabolismo del NO.
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