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La transferencia de átomos de oxígeno desde el nitrito mediado por porfirinas Fe (III) en solución acuosa

Chosu Khin¹, Julie Heinecke, Peter C Ford

¹Department of Chemistry and Biochemistry, University of California, Santa Barbara, California 93106-9510, USA.

Journal of the American Chemical Society

|September 30, 2008

Resumen

El complejo de hierro (III) porfirina FeIII (TPPS) cataliza la transferencia de átomos de oxígeno de nitrito a sustratos, formando complejos de nitrosilo ferroso. En condiciones anaerobias, este proceso finalmente produce óxido nitroso, mostrando una nueva vía catalítica.

Área de la Ciencia:

Química Inorgánica La Química Inorgánica es la química inorgánica.
La catálisis de la catálisis.
Química biomimética es la química biomimética.

Sus antecedentes:

Los complejos de porfirina de hierro son vitales en los sistemas biológicos y la catálisis.
El ion nitrito es una especie clave en varios procesos químicos y biológicos.
Comprender los mecanismos de transferencia de átomos de oxígeno es crucial para el desarrollo de nuevos catalizadores.

Objetivo del estudio:

Para investigar la actividad catalítica del hierro (III) complejo de porfirina FeIII (TPPS) en presencia de nitrito.
Para dilucidar la vía de reacción y los productos de la transferencia del átomo de oxígeno del nitrito a los sustratos.
Explorar el potencial para generar óxido nitroso (N2O) a través de este sistema catalítico.

Principales métodos:

Se reaccionaron soluciones acuosas de FeIII ((TPPS) y iones de nitrito con varios sustratos.
La caracterización del producto implicó la identificación de complejos de nitrosilo ferroso y sustratos oxidados.
Las condiciones de reacción fueron variadas, incluyendo la presencia y ausencia de aire, para estudiar la regeneración y la formación de subproductos.

Principales resultados:

FeIII ((TPPS) y nitrito generaron efectivamente el complejo ferroso de nitrosilo FeII ((TPPS) ((NO) y sustratos oxidados.
Las fosfinas sulfonadas solubles en agua se convirtieron en sus correspondientes monóxidos.
Se observaron tanto la reoxidación aeróbica a FeIII ((TPPS) como la regeneración anaeróbica a las especies férricas (que producen N2O).

Conclusiones:

FeIII ((TPPS) actúa como un catalizador para la transferencia de átomos de oxígeno del nitrito a los sustratos en soluciones acuosas.
La reacción se produce a través de un intermediario de nitrosilo ferroso.
Bajo condiciones anaerobias, el ciclo catalítico da como resultado la formación de óxido nitroso, destacando una nueva vía de generación de N2O.

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