Only negligible uptake was observed for MFI-type samples, indicating that the sizeable TCS molecules cannot diffuse through the 10MR windows. Among the other three zeolites, the highest TCS uptake of 378 mg g -1 was observed for the most Si-rich FAU sample (Si/Al ≈ 400), and both maximum uptake and affinity towards TCS, determined via a Langmuir-Freundlich fit, decreased with decreasing Si/Al ratio. While still being appreciable, uptakes and affinities of BEA-type zeolites (Si/Al ratios from ~80 to ~300) and a MOR-type sample (Si/Al ≈ 110) were lower. In addition to these investigations of synthetic zeolites, TCS adsorption experiments were also performed on natural zeolites (clinoptilolites) modified with organic surfactants, which could be cheaper to produce. It is, however, worth noting that maximal TCS loadings and affinities towards TCS reported in those works were considerably lower than for the bestperforming high-silica zeolites studied by Jiang et al. Computational modelling has become a very widely used tool in zeolite science. Atomistic simulations at different levels of theory have been exploited for various purposes, e.g., to develop a deeper understanding of experimental observations, or to predict properties that were so far not characterized experimentally. With regard to PPCP removal, force field (FF) simulations were employed to compute the adsorption energies of 21 contaminants, including TCS, in all-silica MOR and FAU. Despite the simplistic description of the interatomic interactions, a good correlation between FF adsorption energies and experimental removal efficiencies reported by Rossner et al. was observed. This indicates that such simulations could be employed to predict zeolite adsorbents having a high affinity towards a given PPCP prior to an experimental characterization. Subsequently, the adsorption energies were recomputed using periodic electronic structure calculations in the framework of dispersioncorrected density functional theory (DFT) with the purpose of identifying suitable DFT approaches for the study of functional organic molecules in zeolites. Several earlier DFT studies employed cluster models cut out from the zeolite structure in order to reduce the computational expense, with examples including investigations of sulfonamide antibiotics in all-silica FAU and of salicylic acid, carbamazepine, and ciprofloxacin in cation-exchanged FAU. With ongoing hardware and software developments, periodic calculations are now routinely feasible for unit cells of typical zeolites. A recent DFT investigation studied the adsorption of carbamazepine (CBZ) in eleven all-silica zeolites. In addition to the optimization of CBZ@Zeo adsorption complexes, DFT-based ab initio molecular dynamics (AIMD) simulations were carried out for selected zeolites to analyze the influence of temperature.