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Catalyse photochimie de la réduction du dioxyde de carbone par des porphyrines de fer

Abstract : The transition from fossil fuels to renewable energy sources is a major challenge in today’s society. The first step to address this challenge is to find a way to store and carry this energy, which can be done under the form of chemical bonds through the activation of small molecules like CO2, O2 and H2O. In this context, our work was focused on the catalytic photoreduction of carbon dioxide by three iron porphyrins showing remarkable electrocatalytic properties. We have first studied a homogeneous molecular photochemical approach. A careful analysis of the results, comparing the three porphyrins and the effect of the addition of a weak Brønsted acid, allowed us to propose a reaction mechanism correlating the different behaviour of the porphyrins with their molecular structures. Furthermore, a detailed analysis of the experimental conditions required for the catalysis revealed that they induced the degradation of the porphyrins. To overcome these limits, we studied the use of a photosensitizer, resulting in improved catalytic performances and higher system stability. We also studied a homogeneous molecular photoelectrochemical approach, using p-type Si photoelectrodes. We observed the reduction of CO2 with a photovoltage of 350 mV, thus validating this strategy, but the process is limited by the sensitivity of the photoelectrodes towards O2. We are currently developing new electrodes made of copper oxide to obtain better catalytic performances and a higher stability.
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https://tel.archives-ouvertes.fr/tel-01788373
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Submitted on : Wednesday, May 9, 2018 - 9:03:04 AM
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Mathilde Routier. Catalyse photochimie de la réduction du dioxyde de carbone par des porphyrines de fer. Catalyse. Université Paris Diderot - Paris 7 - Sorbonne Paris Cité, 2014. Français. ⟨tel-01788373⟩

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