Projektbeschreibung
Künstliche Nachahmung der aktiven Stellen von Enzymen und Oberflächen
Das im Rahmen der Marie-Skłodowska-Curie-Maßnahmen finanzierte Projekt MUSYCA zielt darauf ab, unser Verständnis der wichtigen Faktoren auszuweiten, die die Aktivierungsmechanismen von Kohlenstoff-Wasserstoff-Bindungen (C-H-Bindungen) in dinuklearen Kernmaterialien auf Basis von Übergangsmetallen bei Enzymen oder Oberflächen bestimmen. Eines der Hauptziele besteht in der Gewinnung von Komplexen, die M2O-Einheiten enthalten und ausreichend reaktiv sind, um C-H-Bindungen zu oxidieren. Das Projekt wird eine breite Palette von Analyseverfahren einsetzen, um die Reaktivitätsmuster und die entsprechenden Mechanismen zu untersuchen, die der Bildung von M-O-Fragmenten zugrunde liegen sowie bei denen C-O-Bindungen gebildet werden. Es wird auch unsymmetrische Plattformen zur Bildung heterobimetallischer Komplexe entwickeln, um die Synergie zwischen zwei Übergangsmetallen in verschiedenen chemischen Umwandlungsprozessen zu ergründen und zu verstehen.
Ziel
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.
Wissenschaftliches Gebiet
- natural scienceschemical sciencesinorganic chemistryinorganic compounds
- natural scienceschemical sciencesorganic chemistryhydrocarbons
- natural scienceschemical sciencescatalysis
- natural scienceschemical sciencesorganic chemistryaliphatic compounds
- natural sciencesbiological sciencesbiochemistrybiomoleculesproteinsenzymes
Programm/Programme
Thema/Themen
Aufforderung zur Vorschlagseinreichung
Andere Projekte für diesen Aufruf anzeigenFinanzierungsplan
MSCA-IF - Marie Skłodowska-Curie Individual Fellowships (IF)Koordinator
41004 Sevilla
Spanien