GCIS W301/W303 929 E. 57th Street
929 E. 57th Street
Free energy simulations require (i) a method to calculate the potential energy surface (PES), and (ii) a method to sample the potential energy. The “standard model” of computational catalysis uses (i) DFT with some account of dispersion, and (ii) local sampling using harmonic partition functions. Obtaining chemically accurate (± 4 kJ/mol) results requires going beyond the “standard model” in both respects.
We present a general local approach that uses our hybrid QM:QM method (Acc. Chem. Res. 52, 2019, 3502) to calculate CCSD(T)-quality PESs for stationary points, samples the PES locally with anharmonic partition functions (J. Phys. Chem. C 119, 2015, 6128), and uses Grand Canonical Monte Carlo lattice simulations for global sampling over the sites (J. Phys. Chem. Lett.8, 2017, 2713).
We consider adsorption in nanoporous materials, specifically H2O and alkanes in H-zeolites and H2O, CO2, CH4, N2, and CO in metal-organic frameworks.