A Transferable Force Field for Simulating Adsorption in Metal–Organic Frameworks with Open Metal Sites Based on the 12–6–4 Lennard-Jones Potential

Abstract

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.