RUI: SUSCHEM: TOWARDS ACCURATE COMPUTATIONAL DYNAMICAL AND MECHANISTIC STUDIES OF TRANSITION METAL HOMOGENEOUS (PHOTO)CATALYSIS

In this project funded by the Chemical Catalysis Program and the Chemical Theory, Models and Computational Methods Program of the Division of Chemistry, Professor Hendrik Eshuis of Montclair State University is applying and developing computational methods to study the catalysis of chemical reactions using metal complexes and to understand the relationship between the structure of molecules and their activity as catalysts. A computational method, called the Random Phase Approximation Method, is being developed and refined to described fundamental aspects of how chemical bonds are activated by catalysts. This method is also being applied to study how light can drive certain catalysts to perform specific reactions, also known as photocatalysis. This project is contributing to the toolbox of computational methods available for the study of a wide range of chemistries, including catalysis. Ultimately, it may advance the development of more efficient and greener catalysts, a goal of interest to both society and industry. Both undergraduate and graduate students are involved in this research, and Prof. Eshuis is involved in strengthening the computational chemistry component of the chemistry curriculum at Montclair State University.

Prof. Eshuis is applying and developing computational methods to study transition metal homogeneous (photo)catalysis and is primarily focused on the development of the random phase approximation method to describe dynamic and mechanistic aspects of bond activation reactions. The quality of the random phase approximation method is being benchmarked against experimental results and compared to other ab initio and density functional theory methods. The method is being applied to the study of mechanisms of carbon-carbon bond activation reactions by nickel containing catalysts, with a focus on the link between ligand composition and reactivity, as well as in the study of the mechanism of photocatalyzed trifluoromethylation reactions. The random phase approximation method is being further developed to be used in ab initio molecular dynamical studies of mechanisms involving carbon-hydrogen bond activation and extended to open-shell systems.