Accessing the C–C transition state energy on transition metals

Abstract

The search for catalysts that can efficiently convert large hydrocarbons has been an active area of research for decades. To gain insight into those reactions, electronic structure calculations are playing an increasing role but the screening efforts are impeded by the complexity of the reaction networks that can contain hundreds of elementary steps, presenting a large number of computationally expensive transition state barrier calculations. A large number of the sub reactions in the network involve C–C bond dissociation, a step that has been identified as rate determining in many studies. The purpose of this article is to present a methodology that allows for accurate and rapid assessment of transition state energies for C–C bond breaking in any hydrocarbon based on a small number of simple calculations. Our model significantly enhances the capability of expanding the search space for new and efficient catalysts.