Development of a quantum chemistry based conceptual framework for sustainable hydrogenation processes with alkaline-earth metal catalysts (FWOTM977)

Homogenous catalytic hydrogenation of unsaturated compounds, traditionally performed using noble transition metals, is used in countless industrial processes. The quest for a more sustainable society requires finding alternatives for these costly and often harmful precious metals. Recently, simple alkaline-earth-metal catalysts were developed for effective imine and alkene hydrogenation at moderate reaction conditions, breaking the dogma that transition metals are needed for substrate activation. Compared to transition metal catalysis, a good understanding of catalytic hydrogenations mediated by alkaline-earth metals is lacking on both the experimental and the computational side. The main research goal of this project is
providing a conceptual framework facilitating the design of s-block metal complexes for catalytic hydrogenation reactions by combining computational and conceptual techniques. At first, a detailed theoretical investigation of the hydrogenations is required, considering reaction conditions and solvent effects. Once a clear picture of the catalytic mechanism is obtained, conceptual DFT
descriptors, activation-strain analysis and the noncovalent interaction index will allow for conceptualization of the mechanism providing design principles. The role of the metal, substrate functionalization and spectators ligands will be fully rationalized with this novel conceptual framework, constantly coupled to the experimental findings.

Keywords:Homogenous catalysis Catalytic, earth metals

Disciplines:Main group chemistry, Catalysis, Theoretical and computational chemistry not elsewhere classified