(576d) Combining DFT and Kinetic Monte Carlo Simulations to Model Reactions and Transport in MFI Zeolites over Large Time and Length Scales
AIChE Annual Meeting
2021
2021 Annual Meeting
Catalysis and Reaction Engineering Division
In Honor of the 2018 William H. Walker Award Winner I (Invited Talks)
Thursday, November 11, 2021 - 9:00am to 9:20am
Here, we combine density functional theory (DFT) calculations with kinetic Monte Carlo (KMC) simulations to model the formation, diffusion, and isomerization of aromatic species in the MFI framework zeolite in calculations relevant to toluene disproportionation, methylation, and methanol-to-olefins (MTO) processes. DFT is used to calculate activation energies for site-hopping diffusions of aromatics between neighboring MFI intersections via the straight and sinusoidal channels and to calculate free energies of activation and reaction for Brønsted acid catalyzed reactions within these same intersections. The large reaction network consisting of all intracrystalline elementary steps are incorporated into a zeolite-specific kinetic Monte Carlo (KMC) simulation with crystals containing up to 32,000 sites (and four sites per unit cell).