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Regioquímica del tiolato para el intercambio de selenolato y ligando en grupos de oro
Christopher A Hosier1, Christopher J Ackerson1
1Department of Chemistry , Colorado State University , Fort Collins , Colorado 80523 , United States.
Journal of the American Chemical Society
|December 12, 2018
Resumen
Este estudio revela las ubicaciones de los ligandos en los grupos de oro durante las reacciones de intercambio. Muestra una preferencia por ubicaciones específicas de ligandos a lo largo del tiempo, explicando el movimiento de ligandos en superficies de racimo.
Área de la Ciencia:
- Ciencia de los nanomateriales
- Química de las superficies
- Química de coordinación
Sus antecedentes:
- El intercambio de ligandos es crucial para las nanopartículas metálicas, pero la comprensión de su dinámica en los grupos de oro es limitada.
- Los estudios anteriores identificaron múltiples entornos de intercambio, pero carecían de correlación y conocimientos estructurales detallados.
- Los datos estructurales existentes revelaron posiciones para solo una pequeña fracción de los ligandos entrantes.
Objetivo del estudio:
- Para aclarar exhaustivamente los detalles estructurales del intercambio de ligandos en los grupos de oro.
- Para determinar las ubicaciones precisas de los ligandos entrantes durante el intercambio de tiolato a selenolato en racimos de Au25.
- Establecer una base estructural para los mecanismos de intercambio de ligandos en los sistemas de racimos de oro.
Principales métodos:
- Sintetizó y caracterizó 13 estructuras cristalinas de grupos de oro sometidos a intercambio de ligandos.
- Utilizó la cristalografía de rayos X para determinar las posiciones atómicas de los ligandos en la superficie del cúmulo.
- Analizó la distribución y las preferencias de los ligandos tiolato y selenolato a lo largo del tiempo.
Principales resultados:
- Se determinaron las ubicaciones de hasta 17 de los 18 ligandos en grupos de tiolato por selenolato intercambiados Au25(SeR)18-x(SR) x.
- Se observó una preferencia clara y emergente para la colocación de los ligandos tiolados y selenolados.
- Proporcionó los datos estructurales más completos hasta la fecha sobre la dinámica de intercambio de ligandos en grupos de oro.
Conclusiones:
- El estudio proporciona evidencia estructural sin precedentes para los mecanismos de intercambio de ligandos en los grupos de oro.
- Identificó una base estructural para el intercambio de ligandos solvados y la transferencia de ligandos entre grupos.
- Se demostró que el intercambio de ligandos resulta en una traducción neta de ligandos en la superficie del racimo.
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