ED Sciences Chimiques
Bio-inspired catalysis in aqueous droplets: towards a new chemistry of life
by Kevin PEYRAUD-VICRÉ (Acides nucléiques : Régulations Naturelles et Artificielles)
The defense will take place at 14h30 - Amphithéâtre CRPP Centre de Recherche Paul Pascal (CRPP). 115 Avenue du Dr Albert Schweitzer, 33600 PESSAC
in front of the jury composed of
- Valérie DESVERGNES - Directrice de recherche - Université de Bordeaux - Directeur de these
- Emmanuelle MARIE - Directrice de recherche - ENS Paris - Rapporteur
- Estelle MéTAY - Directrice de recherche - Université Claude Bernard, Lyon 1 - Rapporteur
- Nicolas MARTIN - Chargé de recherche - Université de Bordeaux - CoDirecteur de these
- Jean-François BRIèRE - Directeur de recherche - Université de Rouen Normandie - Examinateur
- Olivier MONDAIN-MONVAL - Professeur des universités - Université de Bordeaux - Examinateur
Coacervates are membrane-free aqueous microdroplets formed through liquid–liquid phase separation. They differ from micelles and vesicles in both composition and size. Known for their ability to concentrate enzymes and organic molecules, coacervates can be considered as microreactors or reaction microcompartments. Still largely underexplored in the field of organic chemistry, coacervates offer a unique and original reaction medium for the development of chemical transformations in aqueous solution. This thesis highlights their potential for bio-inspired reactions catalyzed by N-heterocyclic carbenes (NHCs), which are particularly sensitive to the presence of water. We demonstrate that a model Stetter reaction, involving the formation of C–C bonds, can be efficiently carried out in synthetic model coacervates. This approach then led to the design of novel bio-inspired coacervates based on azolium salts, analogous to the natural cofactor thiamine diphosphate, and anions such as ATP, combining compartmentalization with catalytic activation. Other NHC-catalyzed reactions, such as oxidative esterification, were also developed. Altogether, this work presents an integrated and innovative approach to catalysis in aqueous solution, based on the use of self-organized compartmentalized systems.