Investigating the Composition of the Metal Dimer Site in Chabazite for Direct Methane-to-Methanol Conversion

In this paper, we study the complete reaction cycle for methane-to-methanol conversion over various transition-metal dimers in the chabazite zeolite using density functional theory calculations and first-principles-informed microkinetic modelling, building on our previous reaction mechanism for the Cu₂ dimer under dry and wet (with an additional H₂O molecule) conditions. Using the adsorption energy of atomic oxygen as the descriptor, we establish scaling relations for the energy landscapes and generate the volcano plot for reaction rate. Both the first-principles-informed microkinetic model and the volcano plot indicate good activity for the Cu₂, AuPd, and PdCu systems under technologically relevant conditions.

Figure credit: Engedahl, Boje, et al., J. Phys. Chem. C. 2024 (ASAP). doi: 10.1021/acs.jpcc.3c06635.