Computational Screening of Functionalized UiO-66 Materials for Selective Contaminant Removal from Air

Metal–organic frameworks (MOFs) have potential applications for efficient filtration of toxic gases from ambient air. We have used computational methods to examine the efficacy of functionalized UiO-66 with a wide range of functional groups to identify materials suitable for selective adsorption of NH 3, H 2 S, or CO 2 under humid conditions. To this end, adsorption energies at various favorable positions in the structures are obtained from both cluster-based and periodic models. Our cluster calculations show that DFT calculations using the PBE-D2 functional can reliably predict the ranking of materials obtained at the MP2 level. Performing PBE-D2 calculations using periodic models gives rankings of materials that are significantly different from those of cluster calculations, showing that confinement effects are important in these materials. On the basis of these calculations, recommendations for high performing materials are made using PBE-D2 calculations from periodic models that use the full structure of each MOF.