Adsorption of Carbamazepine in All-Silica Zeolites Studied with Density Functional Theory Calculations

14 October 2022, Version 2
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

The anticonvulsant drug carbamazepine (CBZ) is an emerging contaminant of considerable concern due to its hazard potential and environmental persistence. Some previous experimental studies proposed hydrophobic zeolites as promising adsorbents for the removal of carbamazepine from water, but only a few framework types were considered in those investigations. In the present work, electronic structure calculations based on dispersion-corrected density functional theory (DFT) were used to study the adsorption of CBZ in eleven all-silica zeolites having different pore sizes and connectivities of the pore system (AFI, ATS, BEA, CFI, DON, FAU, IFR, ISV, MOR, SFH, SSF framework types). It was found that some zeolites with one-dimensional channels formed by twelve-membered rings (IFR, AFI) exhibit the highest affinity towards CBZ. A “good fit” of CBZ into the zeolite pores that maximises dispersion interactions was identified as the dominant factor determining the interaction strength. Further calculations addressed the role of temperature, performing DFT-based molecular dynamics simulations for selected systems, and of guest-guest interactions between coadsorbed CBZ molecules. In addition to predicting zeolite frameworks of particular interest as materials for selective CBZ removal, the calculations presented here also contribute to the atomic-level understanding of the interaction of functional organic molecules with all-silica zeolites.

Keywords

zeolites
emerging contaminants
density functional theory
adsorption
host-guest-interactions
pharmaceuticals and personal care products (PPCPs)

Supplementary materials

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Supporting Information PDF
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Additional tables and figures
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Sample inputs
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Sample input files for CP2K calculations (structure optimisations and ab-initio MD simulations)
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Data for 1CBZ@Zeo calculations
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Input and output files of calculations for 1CBZ@Zeo configurations (TZVP calculations)
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Data for 2CBZ@Zeo calculations
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Input and output files of calculations for 2CBZ@Zeo configurations (TZVP calculations)
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Results of AIMD simulations, part 1
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Output files of AIMD simulations (PDB trajectories and .ener files) for CBZ and FAU
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Results of AIMD simulations, part 2
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Output files of AIMD simulations (PDB trajectories and .ener files) for MOR and IFR
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