Description du projet
Boucler le cycle du carbone par une conception rationnelle de convertisseurs de CO2 en carburants
Étant donné que la combustion du méthane et d’autres combustibles hydrocarbonés génère des émissions de CO2, le captage de ces émissions pour produire des carburants permet de boucler la boucle et de progresser vers un paradigme de neutralité carbone. Le recyclage du CO2 et de l’H2O en méthane a toujours nécessité des températures et des conditions de réaction très élevées. Récemment, la conversion du CO2 en carburant à l’aide de dispositifs semi-conducteurs à couche mince alimentés par le soleil a suscité un intérêt croissant. Les photocatalyseurs moléculaires offrent des avantages considérables par rapport aux photocatalyseurs inorganiques, toutefois les mécanismes de transfert de charge sont encore mal compris. Le projet SolTIME, financé par l’UE, développera un système photocatalytique innovant qui aidera également les scientifiques à comprendre les mécanismes menant à une conception rationnelle et ouvrant de nouveaux horizons.
Objectif
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.
Champ scientifique
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MSCA-IF - Marie Skłodowska-Curie Individual Fellowships (IF)Coordinateur
43007 Tarragona
Espagne