Flash
Accelerating the discovery of catalysts for the selective oxidation of methane

Selective oxidation of methane to methanol is one of the leading challenges in the global energy demand and commodity supply with the recent booming in shale gas production. Extensive research has been undertaken towards catalyst design to achieve such chemical transformation. On the other hand, methanotrophs have evolved to selectively oxidize methane to methanol using enzymes (e.g., methane monooxygenase) with non-precious metals in the active site. Hence, considerable effort has focused on designing catalyst mimics for selective oxidation of methane to methanol. One commonly employed design principle is 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 ground state intermediates. Nevertheless, it is known that this relationship can break down at single metal sites. Here, we introduce methods to accelerate the characterization of transition states in selective oxidation of methane: the accelerated generation of transition state structures as well as to rapidly converge characterized transition states. We then apply the introduced methods to identify reaction steps where BEP relations hold and where they exhibit enough scatter to mandate transition state characterization. These tools enable the rapid screening of catalysts to uncover new design principles for challenging to catalyze reactions.