A Comprehensive Set of High-Quality Point Charges for Simulations of Metal–Organic Frameworks

Most classical simulations of metal–organic frameworks model electrostatic interactions using point charges on each atom in the structure. We report atomic point charges derived from periodic density functional theory (DFT) electronic structure calculations for more than 2000 unique experimentally synthesized metal–organic frameworks (MOFs). These charges are publicly available as a supplement to the Computation-Ready Experimental MOF database. These DFT-derived atomic point charges are compared to semiempirical group contribution and charge equilibration methods for assigning charges. As an example of using these charges, we examined each MOF for usefulness in the adsorptive removal of tert-butyl mercaptan (TBM) from natural gas. Monte Carlo simulations revealed many candidate MOF structures with high selectivity for TBM over CH4 and high TBM capacity. We anticipate that this public data set of atomic point charges for MOFs will facilitate high-throughput screening for a wide variety of applications in which electrostatic interactions must be considered.