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Complejos de torio mono- y bis (imido) obtenidos por reprotonación de amidas ciclo-metaladas
Nicola L Bell1, Laurent Maron2, Polly L Arnold1
1EaStCHEM School of Chemistry, University of Edinburgh , Edinburgh EH9 3FJ, U.K.
Journal of the American Chemical Society
|August 6, 2015
Resumen
Los investigadores sintetizaron nuevos complejos de torio con dobles enlaces de torio y nitrógeno, avanzando modelos para combustibles nucleares y activación de enlaces C-H. Este trabajo presenta el primer complejo de bis (imido) torio, que ofrece nuevos conocimientos sobre la química de los actinuros.
Área de la Ciencia:
- Química organometálica
- Química inorgánica
- Ciencias de los materiales
Sus antecedentes:
- Los enlaces múltiples actinuro-nitrógeno son cruciales para el desarrollo de combustibles y catalizadores nucleares avanzados.
- Mientras que los enlaces múltiples de uranio-nitrógeno están bien estudiados, los enlaces dobles de torio-nitrógeno siguen siendo raros, siendo los complejos de torio bis (imido) desconocidos anteriormente.
Objetivo del estudio:
- Para sintetizar y caracterizar nuevos complejos de torio mono (imido) y bis (imido).
- Explorar las propiedades estructurales y de enlace de los enlaces dobles tório-nitrógeno.
- Evaluar el potencial de estos complejos como modelos para combustibles nucleares y activación de enlaces C-H.
Principales métodos:
- Reacciones de inserción en el enlace Th-C de las amidas de torio ciclometaladas.
- Análisis de difracción de rayos X para la determinación estructural.
- Métodos computacionales para el análisis de la estructura electrónica y de la unión.
Principales resultados:
- Síntesis exitosa de un nuevo complejo de torio mono (imido), K[Th (NAr) N′′3], y el primer complejo de torio bis (imido), K2[Th (NAr) 2N′′2].
- Los estudios de rayos X y computacionales revelaron una geometría cis-bis (imido), análoga a los metales de transición.
- El análisis indicó bonos ThN polarizados con una orden de bonos Wiberg dos veces mayor que la del bono Th-N único.
Conclusiones:
- La síntesis de complejos de torio bis (imido) expande la química conocida de los enlaces múltiples torio-nitrógeno.
- La geometría y las características de enlace "similares a los metales de transición" observadas proporcionan información valiosa sobre la reactividad de los actinuros.
- Estos hallazgos contribuyen a la comprensión fundamental de los complejos de actinidos para aplicaciones potenciales en la catálisis y el desarrollo de combustible nuclear.
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