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Puntos de polímero como vesículas de membrana fotoactivas para el autoensamblaje de la [FeFe]-hidrogenasa y la

Mariia V Pavliuk¹, Marco Lorenzi², Dustin R Morado³

¹Department of Chemistry─Ångström Laboratory, Physical Chemistry, Uppsala University, 751 20 Uppsala, Sweden.

Journal of the American Chemical Society

|July 21, 2022

Resumen

Este estudio desarrolló un sistema biohíbrido estable utilizando puntos de polímero (Pdots) y HydA1 [FeFe]-hidrogenasa para la producción eficiente de combustible solar a través de la fotosíntesis semiartificial.

Área de la Ciencia:

Biotecnología
Ciencias de los materiales
La fotoquímica

Sus antecedentes:

La fotosíntesis semiartificial requiere fotosensibilizadores estables para impulsar la actividad enzimática para la producción de combustible solar.
Los puntos de polímero (Pdots) ofrecen biocompatibilidad, estabilidad del pH y modificabilidad de la superficie, lo que los convierte en fotosensibilizadores adecuados.
Comprender la interacción entre los fotosensibilizadores y las enzimas es crucial para optimizar los sistemas biohíbridos.

Objetivo del estudio:

Para investigar el ensamblaje biohíbrido de puntos poliméricos binarios (Pdots) y HydA1 [FeFe]-hidrogenasa.
Caracterizar la interacción y la estabilidad de este sistema de enzimas Pdot para la generación de combustible solar.
Para aclarar el mecanismo de recolección de luz, separación de carga y transporte en el sistema biohíbrido.

Principales métodos:

Electroforesis en gel de agarosa, microscopía electrónica de transmisión criogénica (Cryo-TEM) y tomografía electrónica criogénica (Cryo-ET) para confirmar la unión de la enzima.
Espectroscopia transitoria ultrarrápida para analizar los procesos fotoinducidos dentro de los Pdots.
Los ensayos de evolución del hidrógeno cuantifican la eficiencia y la estabilidad de la producción de combustible solar.

Principales resultados:

Se confirmó la unión directa de la HydA1 [FeFe]-hidrogenasa a los Pdots en forma de toroides.
Los Pdots de heterounión con una arquitectura de donante-aceptor lograron una separación de carga por debajo del picosegundo, mejorando la evolución del hidrógeno (88,460 μmolH2·gH2asa−1·h−1).
El ensamblaje biohíbrido demostró estabilidad a largo plazo, con una producción de hidrógeno persistente durante días y un número de volúmenes (TON) de 37.500 ± 1290.

Conclusiones:

Se creó con éxito un sistema biohíbrido estable y homogéneo que combina nanopartículas de polímero y [FeFe]-hidrogenasa.
La interacción Pdot-enzima proporciona información mecanicista sobre la recolección de luz y el transporte de carga para la fotosíntesis semiartificial.
Este enfoque ofrece una vía prometedora para desarrollar sistemas de producción de combustible solar altamente eficientes que superen a las contrapartes naturales y artificiales.

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