Descripción del proyecto
Cerrar el ciclo del carbono con un diseño racional de los convertidores de CO2 en combustible
Dado que la combustión de metano y otros combustibles hidrocarbúricos genera emisiones de CO2, la captura de estas emisiones para producir combustibles cierra un círculo y nos hace avanzar hacia un paradigma de cero emisiones netas de carbono. Tradicionalmente, para reciclar CO2 y H2O y convertirlos en metano, se requerían temperaturas muy elevadas y condiciones de reacción. En los últimos tiempos, la conversión de CO2 en combustible mediante dispositivos solares semiconductores de película fina ha generado un interés creciente. Los fotocatalizadores moleculares ofrecen ventajas significativas sobre los inorgánicos, pero no se conocen bien los mecanismos de transferencia de carga. El equipo del proyecto SolTIME, financiado con fondos europeos, desarrollará un innovador sistema fotocatalítico que además ayudará a los científicos a esclarecer dichos mecanismos, lo cual conducirá a un diseño racional y a nuevos horizontes.
Objetivo
Solar fuels can be synthesized by integrating electrocatalysts with semiconductors, using sunlight to drive endergonic chemical reactions. Employing molecular electrocatalysts allows the tunability, selectivity, and three-dimensional architectures associated with molecular components to be combined with the solar energy capture and conversion properties of solid-state semiconducting materials. However, there is a lack of understanding of how photo-generated carriers are transported through these systems, disfavouring the rational design of efficient photoelectrocatalytic constructs. This proposal aims to interface copper porphyrins with built-in hydroxyl groups, known catalysts for CO2 reduction, to carbon nitride for photo-promoted generation of highly reduced products from CO2, including methane and ethanol. Catalytic activity and selectivity will be studied by using multi-dimensional approaches for porphyrin immobilization, drawing inspiration from the extended coordination spheres crucial in biological tuning of enzymatic activity. This will be achieved through synthesis of three distinct reaction environments at carbon nitride consisting of: a porphyrin monolayer, a polymer film coordinating the porphyrin, and a 2-D highly ordered covalent-organic framework (COF) composed of the porphyrin. It is expected that these specialised environments will give rise to distinct kinetic responses and product distribution. Existing electrochemical models will be extended to this photoelectrochemical data to investigate the interplay of light flux, substrate and electron diffusion, and catalytic rates, leading to the extrapolation of fundamental principles governing interfacial photo-induced charge transfer at catalytic thin films. Through this project, leadership training, language acquisition, and communication skills will be emphasized, furthering the experienced researcher’s career goals and preparing her for an independent career in solar fuels.
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MSCA-IF - Marie Skłodowska-Curie Individual Fellowships (IF)Coordinador
43007 Tarragona
España