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Lograr la detección reversible de nitroxilo mediante la sintonización del entorno de ligandos de los complejos
Sunghee Kim1, Mikael A Minier1, Andrei Loas1
1Department of Chemistry, Massachusetts Institute of Technology , Cambridge, Massachusetts 02139, United States.
Journal of the American Chemical Society
|February 3, 2016
Resumen
Los investigadores exploraron complejos de cobre para detectar nitroxilo (HNO) selectivamente sobre otras moléculas. Un complejo mostró reducción selectiva por HNO, allanando el camino para nuevas sondas fluorescentes.
Área de la Ciencia:
- Química de coordinación
- Detección de sustancias químicas
- Química bioorgánica
Sus antecedentes:
- El nitroxilo (HNO) es una molécula de señalización crucial con una vida útil corta.
- El desarrollo de sondas fluorescentes selectivas para el HNO es un desafío debido a su reactividad y similitud con otras especies reactivas de nitrógeno.
- Las sondas a base de metal ofrecen propiedades redox únicas para aplicaciones de detección.
Objetivo del estudio:
- Investigar los factores que influyen en la selectividad de los derivados de Cu (II) -ciclam (14-N4) para la detección de nitroxilo (HNO).
- Comprender la reactividad de los complejos de cobre con HNO, óxido nítrico (NO), tiolos y sulfuro de hidrógeno (H2S).
- Explorar el potencial de los complejos azamacrocíclicos de cobre en el diseño de nuevas sondas fluorescentes de HNO.
Principales métodos:
- Síntesis y caracterización de cinco derivados del ciclo Cu (II) (14-N4).
- Análisis espectroscópico (UV-vis) para controlar las reacciones con el NO y el HNO generados a partir de la sal de Angeli.
- Mediciones electroquímicas para determinar los potenciales de reducción.
- Preparación y ensayo de un complejo de ligando tia/aza (14-N2S2) mezclado con Cu.
Principales resultados:
- Los complejos de Cu (II) -ciclam no mostraron ninguna reacción con el gas NO.
- [Cu ((II) ((14-N4-Ts) ((OTf)) ] mostró una reducción selectiva de Cu ((II) tras la exposición al HNO, correlacionada con su alto potencial de reducción.
- El complejo Cu (II) -14-N2S2 reaccionó de manera reversible con el HNO pero carecía de selectividad sobre los tiolos y el H2S.
- Los patrones de reactividad proporcionaron información sobre los factores que rigen la selectividad del HNO.
Conclusiones:
- El potencial de reducción de los complejos Cu (II) es un factor clave para lograr la selectividad del HNO.
- Los complejos azamacrocíclicos de cobre muestran potencial para la detección recurrente de HNO.
- Este estudio sienta las bases para el desarrollo de una nueva generación de sondas fluorescentes selectivas basadas en metales para el HNO.
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