Demonstrating and Utilizing [C-H···F-C] and Related Weak Non-Covalent Interactions in Catalysis: Creation of Active Sites with Unusual Peripheral Environments·
DescriptionThe participation of repulsive non-bonded steric interactions and attractive transient contacts are well-established in olefin polymerization reactions, but the concept of weak attractive non-covalent interactions between the growing polymer chain and a functionalized "non-innocent" ancillary ligand is new. Models demonstrating such interactions were recently reported for the first time, and this proposal aims to build upon them by exploring weak polymer‧‧‧ligand interactions as a novel approach towards innovations in polyolefin catalyst design. Synthesis of complexes supported by ligands functionalized with suitable hydrogen-bond acceptor groups will be undertaken. Non-covalent contacts such as weak hydrogen bonds are ideally applicable as attractive ligand‧‧‧polymer interactions, and their tunability paves the way for molecular recognition. The anticipated non-covalent interactions will be investigated by spectroscopic and crystallographic methods, while model compounds displaying these contacts will be developed synthetically and by employing theoretical calculations to guide catalyst design. The generation of unusual environments around the active site along with advances towards new catalytic processes and the generation of novel polymeric materials are envisaged.
|Effective start/end date||1/01/07 → 3/10/11|