(166b) Reaction Mechanism Generation for Predictive Simulations in Catalysis

Quantum chemistry provides a first principles approach to efficiently reveal microscopic details of chemical reactions. These simulations usually start with a chemically intuited hypothesis of a reaction mechanism, followed by atomistic simulation of the proposed reaction sequences. Since this procedure is highly dependent on existing chemical intuition, success is less likely if the reaction mechanism is unusual or complicated in nature.

New tools developed in the Zimmerman group are providing a streamlined method for reaction mechanism prediction. Without requiring the user to hypothesize reaction mechanisms, the tools systematically evaluate a set of plausible reactions for their thermodynamics and kinetics. The results include the lowest energy barrier elementary reaction steps proceeding outward from a set of starting materials. This talk will focus on our methods for transition metal catalyzed reactivity and the use of multiple reagents to form complex multi-step reaction networks. This will involve a detailed discussion of the Single-Ended Growing String Method (J. Comput. Chem. 2015, 36, 601-611), which provides reaction paths and transition states starting from a single intermediate, as well as details of our combinatorial reaction hypothesis generator (J. Comput. Chem. 2013, 34, 1385-1392).