Machine learning potential for modelling dynamic hydrogen bond networks in MOF MIL-120

Abstract

Metal-organic frameworks (MOFs) are porous materials with the potential for gas adsorption and separation technologies due to their tunable structural and chemical characteristics. However, simulating gas adsorption isotherms in MOFs with DFT-level accuracy remains a key challenge. In this work, we use MIL-120 as a case study and propose a comprehensive computational workflow to fine-tune a pre-trained MACE potential, enabling the creation of accurate machine-learning interatomic potentials tailored for frameworks with dynamic structural behavior. Using this ML potential to accelerate sampling, we uncover a strong coupling between CO₂ adsorption and the complex dynamic hydrogen-bond network on the MIL-120 pore surface. The presence of CO₂ induces local configurational rearrangements that reshape the pore environment. This insight provides a generalizable strategy for simulating adsorption in other flexible MOF systems.