Towards Accurate and Scalable High-throughput MOF Adsorption Screening: Merging Classical Force Fields and Universal Machine Learned Interatomic Potentials

Abstract

High-throughput computational screening (HTCS) of gas adsorption in metal-organic frameworks (MOFs) typically relies on classical generic force fields such as the Universal Force Field (UFF), which are efficient but often fail to capture complex host-guest interactions. Universal machine-learned interatomic potentials (u-MLIPs) offer near-quantum accuracy at far lower cost than density functional theory (DFT), yet their large-scale application in adsorption screening remains limited. Here, we present a hybrid screening strategy that merges Widom insertion Monte Carlo simulations performed with both UFF and the PreFerred Potential (PFP) u-MLIP to evaluate the adsorption performance of a large MOF database, using ethylene capture under humid conditions as a benchmark. From a curated set of MOFs, 88 promising candidates initially identified using UFF-based HTCS were re-evaluated with the PFP u-MLIP, benchmarked against DFT calculations to refine adsorption predictions and assess the role of framework flexibility. We show that PFP u-MLIP is essential to accurately assess the sorption performance of MOFs involving strong hydrogen bonding or confinement pockets within narrow pores, effects poorly captured using UFF. Notably, accounting for framework flexibility through full unit cell relaxation revealed deviations in ethylene affinity of up to 20 kJ mol-1, underscoring the impact of guest-induced structural changes. This HTCS workflow identified seven MOFs with optimal pore sizes, high ethylene affinity, and high C2H4/H2O selectivity, offering moisture-tolerant performance for applications from food packaging to trace ethylene removal. Our findings highlight the importance of accurately capturing host-guest energetics and framework flexibility, and demonstrate the practicality of incorporating u-MLIPs into scalable HTCS for identifying top MOF sorbents.