We are studying catalysts that transform non-reactive molecules containing carbon-oxygen and carbon-fluorine bonds into reactive molecules containing carbon-element bonds (element = B, Al, Zn, Mg). These reactive intermediates may undergo further reactions, forming new carbon-carbon and carbon-heteroatom bonds.
The approach will allow the synthetic diversification of simple ethers and fluorocarbons. Hydrodefluorination and hydrodeoxygenation, the transformation of carbon-fluorine and carbon-oxygen bonds to carbon-hydrogen bonds, are important competitive reactions.
The design mold for homogeneous catalysts of rare-earth metals has been set for decades. Catalysts typically incorporate a reactive sigma-bonded substituent and sterically demanding spectator ligands. We recently introduced a group 3 complex that incorporates three elements of ligand design: appended X- and L-type ligands along with reactive sigma-bonded substiutents.
We are studying this complex and related group 3 amides in C-H bond functionalisation and the dehydrogenation of protic and hydridic substrates. We are investigating the role of the supporting ligand in bond activation.
As an undercurrent to our catalytic studies, we are interested in studying the interaction of heavier main group hydrides (M = Al, Zn, Mg) with transition metals. For example, aluminium hydrides have been shown to reversibly coordinate to Zr(IV) and Cu(I) complexes and non-reversibly react with Rh(III) intermediates. We are studying the nature of the bonding in these complexes and not only investigating their role in the catalytic functionalisation of carbon-oxygen and carbon-fluorine bonds but also more broadly in small molecule activation.