Description du projet
Imiter artificiellement les sites actifs des enzymes et des surfaces
Financé dans le cadre du programme d’actions Marie Skłodowska-Curie, le projet MUSYCA entend mieux comprendre les facteurs clés qui régissent les mécanismes d’activation des liaisons carbone-hydrogène (C-H) dans les noyaux dinucléaires à base de métaux de transition présents dans les enzymes ou les surfaces. L’un de ses principaux objectifs est d’obtenir des complexes contenant des entités M2O suffisamment réactives pour oxyder les liaisons C-H. Le projet fera appel à une grande variété de techniques analytiques pour étudier les schémas de réactivité et les mécanismes correspondants qui sous-tendent la formation des fragments M-O et ceux qui impliquent la formation de la liaison C-O. Le projet développera également des plateformes asymétriques pour le développement de complexes hétérobimétalliques afin d’explorer et de comprendre la synergie qui existe entre deux métaux de transition dans différentes transformations chimiques.
Objectif
MUSYCA - Multimetallic Systems for C-H Activation processes - is a project designed to obtain a better understanding of the key factors governing C-H activation phenomena in multinuclear copper-based cores present in the most efficient frameworks such as enzymes or zeolites like methane monooxygenases (MMOs) or Cu-ZSM-5, respectively. One of the main goals of the project is to obtain complexes containing Cu2O entities, which have not yet been interrogated and are reactive enough to oxidize C-H bonds. These will be employed in the stoichiometric and catalytic transformation of hydrocarbon bonds of numerous substrates, from easily convertible to extremely challenging ones, being methane the stretch goal. The reactivity patterns and the corresponding mechanisms underlying the formation of Cu-O fragments as well as those involving the formation of C-O bonds will be studied by using a wide variety of analytical techniques. To this end, robust 2,7-substituted [1,8]naphthyridine scaffolds will be employed as dinucleating ligands, since they resemble the environment surrounding dinuclear active sites in natural enzymes and they facilitate a close interaction between the metals, at the same time that the chelating groups in positions 2 and 7 help to stabilize the resulting complexes. These ligands will also be employed in the other major target of the project, which consists of the development of dinuclear Pt-Cu compounds so as to evaluate the metal cooperativity in a modified Shilov system for C-H activation. Only a few studies have been carried out on the role of copper in the Shilov-type C-H functionalization reaction, showing its great potential for improving the catalytic performance of the active species involved in the process. However, the role of Pt as active catalyst and Cu as oxidant in the same complex has never been investigated, and the aforementioned frameworks developed in the labs of Prof. Tilley are ideal for this purpose.
Champ scientifique
- natural scienceschemical sciencesinorganic chemistryinorganic compounds
- natural scienceschemical sciencesorganic chemistryhydrocarbons
- natural scienceschemical sciencescatalysis
- natural scienceschemical sciencesorganic chemistryaliphatic compounds
- natural sciencesbiological sciencesbiochemistrybiomoleculesproteinsenzymes
Programme(s)
Régime de financement
MSCA-IF - Marie Skłodowska-Curie Individual Fellowships (IF)Coordinateur
41004 Sevilla
Espagne