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CO2 Hidrogenación para formar y ácido fórmico por grupos bimetálicos de paládio-hidruro de cobre

Gaoxiang Liu¹, Patricia Poths², Xinxing Zhang³

¹Department of Chemistry, Johns Hopkins University, 3400 N. Charles Street, Baltimore, Maryland 21218, United States.

Journal of the American Chemical Society

|April 7, 2020

Resumen

Este estudio demuestra por primera vez la hidrogenación catalítica del dióxido de carbono (CO2) utilizando grupos bimetálicos de hidruro de cobre y paladio. Un isómero específico del grupo convierte eficientemente el CO2 en formato, destacando el papel de los isómeros de mayor energía en la catálisis.

Área de la Ciencia:

Química inorgánica
Catálisis
Química computacional

Sus antecedentes:

Los grupos de hidrógeno bimétrico son catalizadores prometedores.
Comprender su interacción con moléculas pequeñas como el CO2 es crucial para desarrollar nuevos procesos catalíticos.
Los estudios anteriores no han explorado la hidrogenación de CO2 por estos sistemas.

Objetivo del estudio:

Investigar la reacción entre los aniones de tetrahidruro de cobre-paladio bimetálico (PdCuH4-) y el dióxido de carbono (CO2).
Identificar los intermedios y productos de la reacción.
Para aclarar el mecanismo catalítico y el papel de los diferentes isómeros.

Principales métodos:

Análisis espectrométrico de masas de los productos aniónicos.
Espectroscopia de fotoelectrones de aniones.
Los cálculos químicos cuánticos.

Principales resultados:

Generación eficiente de un complejo intermedio PdCuCO2H4 y formato/ácido fórmico.
Identificación de las estructuras múltiples de PdCuH4 y PdCuCO2H4.
Se encontró que un isómero PdCuH4- de mayor energía impulsa la hidrogenación de CO2.

Conclusiones:

Este trabajo presenta el primer ejemplo de hidrogenación de CO2 por grupos de hidruro bimetálico.
La actividad catalítica está influenciada por el isómero específico del grupo bimetálico.
La contabilización de los isómeros de mayor energía es crítica para comprender y optimizar la catálisis de clúster.

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