Predictive Kinetics in Homogeneous Catalysis

Computational chemistry is often used to assess reaction mechanisms qualitatively. Catalytic reactions in organometallic chemistry are one frequent area of application – as experimental data can be hard to acquire. Still quantitative predictions of reactivity, i.e. computational kinetics studies of catalysis, are harder to perform, as they require very accurate electronic structure methods. However such calculations are now starting to be possible.

The previously studied hydroformylation of alkenes (Computational Kinetics of Cobalt-Catalyzed Alkene Hydroformylation, Laura E. Rush, P. G. Pringle and J. N. Harvey, Angew. Chem., Int. Ed., 2014, 53, 8672 – 8676) will be the basis of the new work, which purpose is to make much firmer conclusions about turnover-limiting steps of the reaction. Moreover the new aspects of hydroformylation of alkenes (e.g. selectivity) may be investigated. In the framework of this project also other catalytic processes like hydrocyanization will be studied.

The aim of this research project is to develop and use multidisciplinary computational techniques (methods and software) in order to extend the knowledge of mechanisms and kinetics of catalytic reaction in organometallic chemistry. Density functional theory and accurate explicitly-correlated coupled-cluster methods will be used to compute energies of the hydroformylation reactions.