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La transferencia de electrones acoplados a protones impulsa la translocación de protones de largo alcance en sistemas

Emmanuel Odella¹, Brian L Wadsworth¹, S Jimena Mora¹

¹School of Molecular Sciences , Arizona State University , Tempe , Arizona 85287-1604 , United States.

Journal of the American Chemical Society

|August 8, 2019

Resumen

Las moléculas bioinspiradas transportan múltiples protones a través de 16 Å utilizando mecanismos Grotthuss impulsados por redox. Esta investigación avanza en la comprensión de la transferencia de electrones acoplados a protones (PCET) para la fotosíntesis y la catálisis artificiales.

Área de la Ciencia:

Química bioorgánica
Catálisis
La fotosíntesis

Sus antecedentes:

La transferencia de electrones acoplados a protones (PCET) es crucial para la bioenergética y la catálisis, vinculando el transporte de electrones y protones.
Las escalas de longitud y los impactos termodinámicos del transporte de protones en el PCET siguen siendo incompletamente entendidos.

Objetivo del estudio:

Diseñar e investigar moléculas bioinspiradas capaces de transportar protones de largo alcance y reversibles a través del PCET.
Explorar las consecuencias termodinámicas de la translocación de protones en distancias extensas.

Principales métodos:

Diseño y síntesis de nuevas moléculas basadas en benzimidazol con unidades de fenol y ciclohexilimina.
Oxidación y reducción electroquímicas para impulsar la translocación de protones.
Espectroscopia infrarroja para monitorear la llegada y salida de protones.

Principales resultados:

Se ha demostrado la translocación reversible de dos, tres y cuatro protones a distancias de hasta ~16 Å utilizando un mecanismo de tipo Grotthuss.
Confirmado el movimiento de protones a través de la conmutación de potenciales electroquímicos y la observación espectroscópica de una banda de IR a 1660 cm.
Proporcionó información teórica y experimental sobre las escalas de longitud de los procesos PCET.

Conclusiones:

Desarrolló "cables de protones" bioinspirados que imitan aspectos clave del PCET biológico, como en el fotosistema II.
Estableció la viabilidad del transporte de protones de largo alcance en sistemas artificiales.
Los hallazgos tienen implicaciones para el diseño de fotosíntesis artificial, bombas de protones y sistemas catalíticos para la oxidación y reducción del agua.

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