title: DFT-Derived Force Fields for Modeling Hydrocarbon Adsorption in MIL-47(V).
abstract: Generic force fields such as UFF and DREIDING are widely used for predicting molecular adsorption and diffusion in metal-organic frameworks (MOFs), but the accuracy of these force fields is unclear. We describe a general framework for developing transferable force fields for modeling the adsorption of alkanes in a nonflexible MIL-47(V) MOF using periodic density functional theory (DFT) calculations. By calculating the interaction energies for a large number of energetically favorable adsorbate configurations using DFT, we obtain a force field that gives good predictions of adsorption isotherms, heats of adsorption, and diffusion properties for a wide range of alkanes and alkenes in MIL-47(V). The force field is shown to be transferable to related materials such as MIL-53(Cr) and is used to calculate the free-energy differences for the experimentally observed phases of MIL-53(Fe).
authors.affiliation: School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, 311 Ferst Drive NW, Atlanta, Georgia 30332, United States.
authors.forename: Ambarish R
authors.initials: AR
authors.lastname: Kulkarni
authors.affiliation: School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, 311 Ferst Drive NW, Atlanta, Georgia 30332, United States.
authors.forename: David S
authors.initials: DS
authors.lastname: Sholl