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Un intermediario trans-hiponitrito en el acoplamiento reductor y la desoxigenación del óxido nítrico por un complejo

Davide Lionetti¹, Graham de Ruiter¹, Theodor Agapie¹

¹Division of Chemistry and Chemical Engineering, California Institute of Technology , 1200 East California Boulevard, MC 127-72, Pasadena, California 91125, United States.

Journal of the American Chemical Society

|March 31, 2016

Resumen

Los investigadores lograron el acoplamiento reductor de óxido nítrico (NO) utilizando un complejo de ítrio-tricobre. Este proceso genera hiponitrito, un intermediario clave para reducir el NO a óxido nitroso (N2O) y nitrógeno (N2).

Área de la Ciencia:

Química inorgánica
Catálisis
Química del medio ambiente

Sus antecedentes:

La reducción del óxido nítrico (NO) es crucial para los procesos biológicos y el control de la contaminación.
El hiponitrito (N2O2(2-)) es un intermediario propuesto en la reducción de NO.
Los nuevos modos de coordinación de la hiponitrita son esenciales para comprender las vías de transformación del NO.

Objetivo del estudio:

Para investigar el acoplamiento reductor de NO utilizando un complejo de ítrio-tricobre.
Caracterizar la formación y coordinación de un intermediario de trans-hiponitrito.
Demostrar el papel del hiponitrito en la reducción del NO a N2O y N2.

Principales métodos:

Síntesis y caracterización de un complejo itrio-tricobre.
Acoplamiento reductivo del óxido nítrico (NO) con el complejo itrio-tricobre.
Reacción del intermediario hiponitrito con los ácidos de Brønsted.
Análisis de los productos de reducción (N2O y N2).

Principales resultados:

Se generó una nueva fracción de trans-hiponitrito, soportada por un núcleo μ-O-bimetálico (Y,Cu) único.
El complejo de hiponitrito produjo con éxito óxido nitroso (N2O) al reaccionar con ácidos de Brønsted.
El complejo itrio-tricobre facilitó la reducción completa de NO a N2 a través del intermedio hiponitrito, utilizando equivalentes reductores almacenados.

Conclusiones:

El complejo itrio-tricobre media efectivamente el acoplamiento reductor de NO para formar un intermediario hiponitrito aislable.
Este estudio valida el complejo de hiponitrito como un intermediario viable en la reducción biológica y ambiental de NO a N2O.
Los hallazgos destacan la utilidad de combinar ácidos de Lewis y metales redox-activos para complejas transformaciones de múltiples electrones.

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