Selective oxidation of short chain hydrocarbon compounds is one of the leading challenges in the global energy demand and commodity supply. Extensive research has been undertaken towards catalyst design to achieve such chemical transformation. On the other hand, Nature has devised the most effective catalysts for selective oxidation of methane to methanol based on non-precious metals using O<sub>2</sub> as the oxidant (e.g., methane monooxygenase).  Hence, considerable effort has focused on designing catalyst mimics for selective and efficient oxidation of short chain hydrocarbons to oxygenates. Computational catalyst design often leverages relationships known as the Bell-Evans-Polanyi (BEP) principle, which connects reaction enthalpy to activation energy, enabling the rapid screening of catalysts based solely on properties of the intermediates. Nevertheless, it is known that this relationship can break down at single metal sites. Here, we describe methods to accelerate the characterization of transition states in selective oxidation of methane. We identify reaction steps where BEP relations hold and where they exhibit enough scatter to mandate transition state characterization. We develop tools for the accelerated generation of transition state structures as well as to rapidly converge characterized transition states. These tools enable the rapid screening of catalysts to uncover new design principles for challenging to catalyze reactions.

Accelerated design of catalysts for the selective oxidation of methane to methanol

2019 Spring National Meeting

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.