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AbstractAbstract
[en] The criticality of global warming urges for the advancement of science to reduce carbon dioxide (CO2) emissions in the atmosphere. At the heart of this challenge is the development of sustainable catalysts that can help capture, activate, reduce, and eventually valorize CO2. This PhD work tried to respond to this call by developing molecular mimics inspired by natural systems in the larger scheme of artificial photosynthesis. Firstly, it involved tracking the journey of a photon of visible light and how it is transformed to a reducing power able to reduce CO2. Secondly, in search for more efficient and stable catalysts, new mimics were synthesized inspired by the exceptional performance of CO dehydrogenase enzymes (CODH) in reducing CO2. Lastly, further understanding of CODH also led to a proof-of-concept that directly valorizes the photo-produced CO for the synthesis of isotopically-labelled amide bonds, a common motif in pharmaceutically-relevant drugs. (author)
[fr]
La criticite du rechauffement climatique incite a chercher des solutions pour reduire les emissions de dioxyde de carbone (CO2). Le developpement de catalyseurs qui peuvent aider a capturer, activer, reduire et valoriser le CO2 est au coeur de ce defi. Cette these a repondu a cet appel en developpant des mimetismes moleculaires inspires de la Nature, dans le cadre plus large de la photosynthese artificielle. Au debut il s'agissait de suivre le parcours d'un photon de lumiere visible et de determiner comment il peut reduire la molecule de CO2. Ensuite afin de realiser des catalyseurs plus efficaces, de nouvelles molecules ont ete synthetisees en s'inspirant de l'enzyme CO deshydrogenase (CODH) qui presente des performances exceptionnelles pour la reduction du CO2. Enfin, une autre propriete du CODH a conduit a une validation de principe pour la valorisation immediate du CO photo-produit dans la synthese des liaisons amides marques, une caracteristique courante des medicaments.Original Title
Strategies bio-inspirees pour la reduction catalytique et la valorisation du dioxyde de carbone
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20 Sep 2019; 217 p; 292 refs.; Available from the INIS Liaison Officer for France, see the INIS website for current contact and E-mail addresses; Chimie
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Thesis/Dissertation
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