Identification of adsorption sites for CO₂ in a series of rare‐earth and Zr‐based metal‐organic frameworks

The adsorption of CO₂ in MOF-808, NU-1000 and a series of rare-earth CU-10 analogues has been studied with first principles DFT and classical Monte-Carlo methods. DFT calculations describe the interaction of CO₂ with the different metal-organic frameworks (MOFs) as physisorption, but where we can distinguish several adsorption sites in the vicinity of the metal nodes. Beyond the identification of adsorption sites, the MOFs were synthesized, activated, and characterized to evaluate their experimental N₂ and CO₂ adsorption capacity. Classical Grand Canonical Monte-Carlo (GCMC) simulations for the adsorption of CO₂ are in very good agreement with DFT results for identifying the most favored adsorption sites in the MOFs. In contrast, a rather mixed agreement between GCMC simulations and experimental results is found for the estimation of adsorption capacity of several MOFs studied toward N₂ and CO₂.