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Mecanismo catalítico único para electrodos intermetálicos ternales cargados con Ru para la síntesis de amoníaco

Yutong Gong¹, Hongchen Li¹, Jiazhen Wu^2,3

¹State Key Laboratory of Solidification Processing, School of Materials Science and Engineering, Northwestern Polytechnical University, Xi'an, Shaanxi 710072, People's Republic of China.

Journal of the American Chemical Society

|May 4, 2022

Resumen

Los electrodos intermetálicos terneros mejoran los catalizadores de rutenio para la síntesis de amoníaco. El rutenio soportado por LaCoSi demuestra una actividad y durabilidad superiores, impulsadas por estructuras electrónicas únicas que promueven la disociación del nitrógeno.

Área de la Ciencia:

Ciencias de los materiales
Catálisis
Química Física

Sus antecedentes:

Los electrodos intermetálicos son componentes catalizadores prometedores para la síntesis de amoníaco y la activación de CO2.
El mecanismo de función preciso de estos electridos sigue siendo poco conocido, lo que limita el desarrollo del catalizador.

Objetivo del estudio:

Sintetizar y evaluar los electridos intermetálicos ternales La-TM-Si (TM = Co, Fe, Mn) como soportes para los catalizadores de rutenio (Ru) en la síntesis de amoníaco.
Aclarar la influencia del metal de transición (TM) en el rendimiento catalítico y comprender el mecanismo subyacente.

Principales métodos:

Síntesis de electridos ternarios intermetálicos La-TM-Si.
Preparación de catalizadores con apoyo de rutenio (Ru) (Ru/La-TM-Si).
Pruebas de actividad catalítica y durabilidad de la síntesis de amoníaco.
Cálculos basados en principios para investigar la estructura electrónica y las vías de reacción.

Principales resultados:

La actividad catalítica siguió el orden Ru/LaCoSi > Ru/LaFeSi > Ru/LaMnSi, con Ru/LaCoSi mostrando una mayor durabilidad.
Se observó una menor energía de activación aparente de N2 en comparación con los catalizadores de Ru convencionales, lo que indica una mayor disociación de N2.
La formación de NH3 en los sitios La fue favorecida energéticamente, evitando potencialmente las relaciones de escala tradicional.
El paso determinante de la velocidad se identificó como la formación de NH2, influenciada por el efecto del metal de transición en las interacciones entre el metal y el soporte.

Conclusiones:

Los electridos intermetálicos terneros, en particular LaCoSi, sirven como huéspedes efectivos para los catalizadores Ru en la síntesis de amoníaco.
La estructura electrónica única y la configuración atómica de estos electridos promueven significativamente la disociación del N2.
El metal de transición (TM) juega un papel crucial en el ajuste de la interacción entre el metal y el soporte y el rendimiento catalítico general.
Estos hallazgos ofrecen una vía para diseñar anfitriones de catalizadores avanzados para la síntesis de amoníaco y las reacciones de hidrogenación.

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