Descrizione del progetto
Imitare artificialmente i siti attivi di enzimi e superfici
Finanziato nell’ambito del programma di azioni Marie Skłodowska-Curie, il progetto MUSYCA cerca di aumentare la comprensione dei fattori chiave che governano i meccanismi di attivazione del legame carbonio-idrogeno (C-H) nei nuclei dinucleari a base di metalli di transizione presenti negli enzimi o nelle superfici. Uno degli obiettivi principali è quello di ottenere complessi contenenti entità M2O che siano abbastanza reattivi da ossidare i legami C-H. Il progetto farà ricorso a un’ampia varietà di tecniche analitiche per studiare i modelli di reattività e i corrispondenti meccanismi alla base della formazione di frammenti M-O e quelli che coinvolgono la formazione del legame C-O. Svilupperà anche piattaforme asimmetriche per lo sviluppo di complessi eterobimetallici per esplorare e comprendere la sinergia tra due metalli di transizione in diverse trasformazioni chimiche.
Obiettivo
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.
Campo scientifico
- natural scienceschemical sciencesinorganic chemistryinorganic compounds
- natural scienceschemical sciencesorganic chemistryhydrocarbons
- natural scienceschemical sciencescatalysis
- natural scienceschemical sciencesorganic chemistryaliphatic compounds
- natural sciencesbiological sciencesbiochemistrybiomoleculesproteinsenzymes
Programma(i)
Argomento(i)
Meccanismo di finanziamento
MSCA-IF - Marie Skłodowska-Curie Individual Fellowships (IF)Coordinatore
41004 Sevilla
Spagna