This proposal addresses currently unresolved fundamental questions concerning the activation and functionalization in homogeneous catalysis of challenging, inherently unreactive substrates like NH3, CO2 or water. Responsive ligands in combination with earth-abundant first row transition metals may hold the key to selective bifunctional activation of these small molecules. This innovative, bioinspired concept, utilizing ligand-metal cooperativity to enhance, tune and control the reactivity of base metals, mimics and circumvents the use of expensive and/or toxic 2nd and 3rd row transition metals. A comprehensive tool-box of readily accessible smart ligand systems with cooperative, redox noninnocent or adaptive features will be used for stoichiometric and ultimately catalytic reactivity studies with Fe, Co, Ni and Cu. This will result in mechanistic understanding of novel pathways for selective N-H and O-H activation on well-defined mono- and dinuclear cooperative complexes. Coupling and insertion reactions with alkenes to yield efficient C-N and C-O bond forming processes and CO2 functionalization will be investigated. This fundamental knowledge is then applied for unprecedented cooperative catalysis with first row transition metals. The project will ultimately result in important leads for the direct intermolecular hydroamination of alkenes, including with ammonia, which is one of the top-ten challenges in catalysis, and the efficient, sustainable production of carboxylic acids from CO2 and alkenes. Also relevant contributions to the oxidative activation of water for hydration reactions with alkynes are foreseen. When successful, my initiatives will enable significant breakthroughs in the design of unique, smart ligand systems for the cooperative activation and functionalization of small molecules with base metals. An ERC starting grant greatly strengthens my position in the emerging field of cooperative homogeneous catalysis.
Fields of science
Call for proposal
See other projects for this call