Gas adsorption and framework flexibility of CALF-20 explored via experiments and simulations.

In 2021, Svante, in collaboration with BASF, reported successful scale up of CALF-20 production, a stable MOF with high capacity for post-combustion CO capture which exhibits remarkable stability towards water. CALF-20's success story in the MOF commercialisation space provides new thinking about appropriate structural and adsorptive metrics important for CO capture. Here, we combine atomistic-level simulations with experiments to study adsorptive properties of CALF-20 and shed light on its flexible crystal structure. We compare measured and predicted CO and water adsorption isotherms and explain the role of water-framework interactions and hydrogen bonding networks in CALF-20's hydrophobic behaviour. Furthermore, regular and enhanced sampling molecular dynamics simulations are performed with both density-functional theory (DFT) and machine learning potentials (MLPs) trained to DFT energies and forces. From these simulations, the effects of adsorption-induced flexibility in CALF-20 are uncovered. We envisage this work would encourage development of other MOF materials useful for CO capture applications in humid conditions.