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Reducción impulsada por el sol de protones acuosos acoplados a la oxidación selectiva de alcohol con un sistema de

Hatice Kasap¹, Christine A Caputo¹, Benjamin C M Martindale¹

¹Christian Doppler Laboratory for Sustainable SynGas Chemistry, Department of Chemistry, University of Cambridge , Lensfield Road, Cambridge CB2 1EW, U.K.

Journal of the American Chemical Society

|June 24, 2016

Resumen

Este estudio presenta un nuevo sistema impulsado por la energía solar para producir combustible de hidrógeno y aldehídos valiosos a partir de agua y sustratos orgánicos. El fotocatalizador sin metales preciosos ofrece una producción química eficiente y sostenible.

Área de la Ciencia:

Fotocatálisis
Energía renovable
Química ecológica

Sus antecedentes:

La división solar del agua es crucial para la producción de combustible de hidrógeno, pero a menudo es ineficiente.
La oxidación del agua produce oxígeno, lo cual es indeseable.
Se necesitan métodos alternativos que combinen la generación de hidrógeno con la síntesis de productos valiosos.

Objetivo del estudio:

Desarrollar un nuevo sistema fotocatalítico para la generación simultánea de H2 y la oxidación del sustrato orgánico.
Para utilizar un nitruro de carbono funcionalizado con cianamida ((NCN) CNx) y un catalizador de níquel (NiP).
Lograr altos rendimientos de productos de valor añadido en condiciones suaves.

Principales métodos:

Irradiación del catalizador (NCN) CNx y NiP en una solución acuosa con un sustrato de alcohol bencílico.
Análisis de la producción de H2 y aldehído mediante cromatografía de gases y líquidos.
Caracterización de las propiedades electrónicas del fotocatalizador mediante espectroscopia de absorción transitoria.

Principales resultados:

El sistema (NCN) CNx-NiP produjo eficientemente H2 y aldehídos en una estequiometría 1:1.
Se observó una alta actividad: 763 μmol (g CNx) para la producción de H2/aldehído, 76 h para la frecuencia de rotación basada en Ni y un 15% de eficiencia cuántica externa.
El sistema demostró estabilidad durante 24 horas y superó a un análogo basado en platino.

Conclusiones:

El sistema de fotosíntesis artificial desarrollado ofrece una vía sostenible y eficiente para producir tanto combustible solar como productos químicos valiosos.
La fotoactividad se atribuye a la oxidación eficiente del sustrato por (NCN) CNx, lo que lleva a electrones atrapados de larga vida.
Este sistema no tóxico y libre de metales preciosos exhibe una economía atómica del 100% y genera dos productos de valor añadido.

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