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Un complejo de amido de hierro progenitor en la catálisis de la oxidación del amoníaco

Yongxian Li¹, Jia-Yi Chen², Qiyi Miao^3,4

¹School of Chemistry and Chemical Engineering, Shandong University, Jinan 250100, China.

Journal of the American Chemical Society

|March 2, 2022

Resumen

Los investigadores desarrollaron un nuevo complejo de amina férrica para la oxidación electrocatalítica del amoníaco. Este sistema permite la formación de hidrazina a través de un mecanismo único que involucra un intermediario Fe ((IV) -amido.

Área de la Ciencia:

Química inorgánica
La electroquímica
Catálisis

Sus antecedentes:

Los complejos de amido son intermedios clave en las transformaciones de amoníaco.
La oxidación electrocatalítica del amoníaco es esencial para la síntesis química a base de nitrógeno.

Objetivo del estudio:

Informar de un sistema de amina férrica bien definido para la oxidación electrocatalítica del amoníaco.
Aislar y caracterizar los intermediarios clave en el mecanismo de oxidación del amoníaco.

Principales métodos:

Síntesis y caracterización de un complejo de aminas férricas [Cp*Fe(1,2-Ph2PC6H4NH) ((NH3) ]+.
Estudios electrocatalíticos para determinar el potencial de oxidación del amoníaco.
Aislamiento y caracterización estructural de Fe ((IV) -amido y especies relacionadas.

Principales resultados:

Se sintetizó un complejo de amina férrica, [1-NH3]+, y se demostró la oxidación electrocatalítica del amoníaco a N2 y H2 a potenciales leves.
Se aislaron y caracterizaron estructuralmente por primera vez una especie formal de Fe ((IV) -amido, [1-NH2] +, y su ácido conjugado [1-NH3] 2+.
Los estudios de mecanismo revelaron que la oxidación de [1-NH2] + conduce a la reacción de la unidad amido con NH3, formando hidrazina.

Conclusiones:

El ligando de fenilamido no inocente facilita la transferencia concertada de un protón y dos electrones, lo que lleva a la formación de hidrazina.
Este trabajo proporciona nuevos conocimientos sobre el mecanismo de oxidación del amoníaco y la síntesis de hidrazina utilizando complejos de hierro bien definidos.

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