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Conversión ascendente de aniquilación de tripletes por infrarrojos cercanos de alta eficacia para la catálisis

Ling Huang¹, Wenting Wu², Yang Li¹

¹Department of Biochemistry and Molecular Pharmacology, University of Massachusetts Medical School, Worcester, Massachusetts 01605, United States.

Journal of the American Chemical Society

|October 19, 2020

Resumen

Los investigadores desarrollaron un nuevo método para mejorar los sistemas orgánicos de conversión ascendente de aniquilación de tripletes (TTA-UC) utilizando luz de infrarrojo cercano (NIR). Este avance mejora la eficiencia de TTA-UC para aplicaciones en biología, energía solar y fotocatálisis.

Área de la Ciencia:

Ciencias de los materiales
La fotoquímica
Productos electrónicos orgánicos

Sus antecedentes:

La conversión orgánica por aniquilación de tripletes (TTA-UC) es prometedora para diversas aplicaciones, incluida la biología, la energía solar y la fotocatálisis.
El desarrollo de sistemas TTA-UC eficientes que puedan activarse con luz de infrarrojo cercano (NIR) sigue siendo un desafío importante.

Objetivo del estudio:

Adaptar sistemáticamente las moléculas del aniquilador para sistemas TTA-UC altamente eficientes que puedan activarse mediante NIR.
Investigar el impacto de la modificación de las energías de estado excitado triplet y singlet en el rendimiento de TTA-UC.

Principales métodos:

Modificaciones químicas de un aniquilador de perileno para crear derivados con energías de estado excitado triplet (T₁) y singlet (S₁) a medida.
Ajuste del sistema TTA-UC de procesos endotérmicos a exotérmicos.
Evaluación de la eficiencia de la conversión al alza junto con el fotosensibilizador PdTNP bajo irradiación de luz NIR.

Principales resultados:

Se logró una eficiencia de conversión al alza del 14,1% utilizando un derivado óptimo de perileno (100 μM) con PdTNP (10 μM) bajo luz NIR de baja potencia (100 mW/cm2, 720 nm).
Se ha demostrado la catálisis fotorredóxica impulsada por la luz NIR utilizando el sistema TTA-UC desarrollado, superando las reacciones impulsadas por la luz visible.
Se demostró la operabilidad de la catálisis fotorredóxica mediada por TTA-UC al aire libre.

Conclusiones:

El estudio presenta una estrategia exitosa para mejorar la conversión orgánica activable por NIR a través de la adaptación sistemática del aniquilador.
El sistema TTA-UC desarrollado ofrece un up-shifter de longitud de onda de luz altamente eficaz para la fotocatálisis impulsada por NIR, superando las limitaciones de profundidad de penetración.
Este avance allana el camino para aplicaciones más amplias previamente obstaculizadas por materiales ineficientes de TTA-UC.

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