Methanol oxidation to formaldehyde on VSiBEA zeolite: a combined DFT/vdW/transition path sampling and experimental study

Density functional calculations have been performed applying periodic boundary conditions to investigate the oxidation of methanol on vanadium-containing SiBEA zeolite (VSiBEA). Different types of reaction configurations have been set up in conformity with the experimental conditions. Thermodynamic property calculations for T > 0 K have been performed and compared with the available experimental results. Transition path sampling was employed to unravel the reaction mechanisms for oxidation of methanol on vanadium-containing SiBEA zeolites at three temperatures (300, 415, and 523 K). Dispersion interactions were accounted for by adding a damped dispersion term to the PBE energies. The study of different reaction pathways was combined with experimental data that enabled us to shed more light on the reaction mechanism.