A Transferable Force Field for Simulating Adsorption in Metal-Organic Frameworks with Open Metal Sites Based on the...

Metal-organic frameworks (MOFs) that contain coordinatively unsaturated open metal sites (OMSs) provide strong host-guest interactions, making them promising sorbents for low-concentration gas adsorption applications such as direct air capture and atmospheric water harvesting. However, accurately modeling host-guest interactions involving OMSs remains challenging for classical force fields (FFs) based on the 12-6 Lennard-Jones (LJ) potential, as the polarization effect of the guest molecule induced by the positively charged OMS is not considered. Here, we introduce an FF based on the 12-6-4 LJ potential, which incorporates charge-induced dipole interactions and is parametrized against a diverse set of host-guest potential energy surfaces (PESs) obtained from density functional theory (DFT). The resulting FF, trained on a generic trimetallic cluster, performs well in both host-guest binding energetics and gas adsorption isotherms across different OMS-containing MOFs, including MOF-74 series and Cu-BTC. These results highlight the excellent transferability of our approach and its potential to enhance the accuracy and robustness of high-throughput MOF discovery workflows, particularly for gas adsorption and separation in large and diverse MOF databases.