Fully Computational Lead-Development of Fluoro-Olefin Polymerization Catalysts

Abstract

Coordinative polymerization of fluorinated olefins is still a challenging task. We analyzed the catalytic properties of diimido chromium VI compounds computationally by density functional methods. It was found that reactivity predictions depend strongly on the density functional chosen for the computations. Therefore, DFT calculations were calibrated to high level wave function theory calculations. Then geometrical parameters, which can be tuned by a ligand, were scanned to elucidate their influence on the catalytic activity. Having arrived at an optimal parameter set, we randomly assembled chromium complexes from a fragments database and automatically checked for their activities. This led to the proposal of three exemplary catalyst candidates.

How to Modulate Catalytic Properties in Nanosystems: The Case of Iron–Ruthenium Nanoparticles

“…More extensive virtual screening and de novo design procedures, more typically used in the development of pharmaceuticals, are starting to be used in catalyst discovery/optimization. One of the first studies in which this methodology was employed was reported by Burger et al 44. and focused on Cr VI –diimido‐catalyzed fluoroalkene polymerizations.…”

An Evolutionary Algorithm for de Novo Optimization of Functional Transition Metal Compounds

“…A de novo approach to predict the ground state coordination isomers of a subclass (trigonal bipyramidal) of transition metal complexes using a hierarchy of molecular-level computational methods has been reported . Similarly, automated molecular builders handling subclasses of metal chelate complexes also exist. , It is also encouraging that much progress has been made in the use of molecular-level computational methods for prediction of homogeneous catalysts in recent years, with a clear tendency toward the adoption of powerful quantitative structure–activity relationships (QSAR) and other computerized techniques to get the most out of the data. − All of these advances together suggest that the field is ready to explore the potential of a fully integrated drug-design-like de novo approach to design of catalysts and other molecular inorganic compounds.…”