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Inserción y escisión de dinitrógeno por un grupo de tricobalto enlazado metal-metal
Mary C Eaton1, Vincent J Catalano2, Jason Shearer3
1Center for Catalysis and Florida Center for Heterocyclic Compounds, Department of Chemistry, University of Florida, Gainesville, Florida 32611-7200, United States.
Journal of the American Chemical Society
|April 8, 2021
Resumen
Los investigadores redujeron un grupo de bromuro de cobalto, formando un grupo de cobalto. Este racimo se une al dinitrógeno, lo que lo activa para su posterior escisión en tris ((trimetilsilil) amina. Este estudio avanza en la química de la fijación del nitrógeno.
Área de la Ciencia:
- Química inorgánica
- Química organometálica
- Ciencias de los materiales
Sus antecedentes:
- Los grupos de cobalto son de interés para la catálisis y la fijación de nitrógeno.
- Los complejos metálicos soportados por ciclófano ofrecen entornos estéricos y electrónicos únicos.
- La comprensión de las interacciones metal-ligando es crucial para el diseño de nuevos catalizadores.
Objetivo del estudio:
- Síntesis y caracterización de un nuevo cúmulo de tricobalto.
- Para investigar la reactividad de este grupo con el nitrógeno.
- Para explorar el potencial de la escisión del nitrógeno y la funcionalidad.
Principales métodos:
- Síntesis de un grupo de bromuro de tricobalto.
- Reducción electroquímica para formar un grupo de cobalto.
- Reacción con dinitrógeno y posterior reducción.
- Cálculos de la teoría funcional de la densidad (DFT) para el análisis de la estructura electrónica.
- Caracterización espectroscópica (por ejemplo, espectroscopia IR).
Principales resultados:
- Formación de un grupo de 48 electrones de Co3 (I) (2) a través de la reducción y la pérdida de haluros.
- Incorporación de dinitrógeno en la cavidad del racimo formando complejo (3) con enlaces metales-metales rotos.
- Los cálculos de DFT indicaron un orden N-N de 2,1 para el dinitrógeno unido.
- La reducción subsiguiente del complejo (3) condujo a la escisión de N2, dando lugar a la tris ((trimetilesil) amina.
Conclusiones:
- El cúmulo de cobalto sintetizado puede activar y dividir el nitrógeno.
- Se caracterizó la estructura electrónica del ligando de dinitrógeno.
- Este trabajo demuestra una vía para la fijación y la funcionalización del nitrógeno utilizando complejos de cobalto.
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