Simulation-based evaluation of zeolite adsorbents for the removal of emerging contaminants

Fischer, Michael

doi:10.1039/d0ma00025f

Cited by 32 publications

(43 citation statements)

References 81 publications

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“…Molecular structures of 21 organic contaminants were taken from earlier work. [19] Table 2 lists these contaminants, including sum formula, molecular weight, and typical applications. The structures had been obtained from the PubChem [71] and CheBi [72] databases, and were preoptimised with the DREIDING force field.…”

Section: Models Of Organic Contaminants Zeolites and Adsorption Compl...mentioning

confidence: 99%

“…Likewise, the structure models of all-silica MOR and FAU were the same as in earlier work. [19] These models were taken from the IZA Database [2] and optimised using the force field of Sanders, Leslie, and Catlow (SLC), [73] which has been shown to give good agreement with experimental structure data for all-silica zeolites. [74,75] Whereas the regular unit cell was used for FAU, a 1×1×3 supercell was employed for MOR.…”

Section: Models Of Organic Contaminants Zeolites and Adsorption Compl...mentioning

confidence: 99%

“…Recent work showed a good correlation between zeolite-guest interaction energies and experimentally observed removal efficiencies for 21 organic contaminants in MOR-and FAU-type zeolites. [19] The interaction energies were computed using a very simplistic approach based on Monte Carlo (MC) simulations and subsequent energy minimisations with the DREIDING force field (FF), [20] indicating that even relatively crude simulations could be very useful to identify adsorbent-guest combinations of interest. Other authors have employed FFbased molecular dynamics (MD) simulations to study the diffusion of pharmaceuticals through zeolite structures in the context of drug delivery investigations.…”

Section: Introductionmentioning

confidence: 99%

“…Due to the well-known shortcomings of standard DFT in describing long-range dispersion interactions, which play an important role for adsorption phenomena, recent investigations have usually employed dispersion-corrected "flavours" of DFT. For example, the DREIDING calculations carried out in one of the aforementioned studies [19] were supplemented by DFT calculations using the Perdew-Burke-Ernzerhof (PBE) [27] functional with a D3 dispersion correction [28] functional for selected systems. It was shown that FF and DFT give, by and large, the same trends, validating the conclusions drawn from the DREIDING calculations.…”

Section: Introductionmentioning

confidence: 99%

“…In Part 1, adsorption energies are computed for a variety of organic contaminants in two allsilica zeolites (MOR and FAU), with the choice of adsorbents and adsorbates following previous experimental and computational work. [6,19] In addition to evaluating the differences in absolute adsorption energies, it is also assessed whether different functionals deliver any appreciable differences in the relative trends. It should be emphasised that this work does not attempt to obtain DFT-computed adsorption energies that could be directly compared to any observable quantity.…”

Section: Introductionmentioning

confidence: 99%

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Studying the adsorption of emerging organic contaminants in zeolites with dispersion-corrected density functional theory calculations: From numbers to recommendations

Fischer

2022

Preprint

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It has been established that adsorption energies obtained from dispersion-corrected density functional theory (DFT) calculations show a considerable dependence on the choice of exchange-correlation functional and dispersion correction. A number of investigations have employed different approaches to compute adsorption energies of small molecules like methane, ethane, or carbon dioxide in different types of zeolites (all-silica, protonated, cation-exchanged), using reference values from high-level calculations and/or experiments. Such comparative studies are lacking for the adsorption of larger functional organic molecules such as pharmaceuticals or personal care products in zeolites, despite the potential relevance for various applications, among them contaminant removal and drug delivery. The present study aims to fill this gap by comparing adsorption energies and, for selected cases, equilibrium structures of adsorption complexes of emerging organic contaminants in all-silica zeolites, employing a total of 13 dispersion-corrected DFT approaches. Methods using a pairwise (D3) dispersion correction as well as non-local van der Waals density functionals were included. A comparison of adsorption energies obtained for a variety of emerging organic contaminants in zeolites with the MOR and FAU topologies showed that the absolute values vary widely, whereas the qualitative trend across the set of zeolite-contaminant combinations are not strongly dependent on the choice of functional. For a few cluster models, DFT adsorption energies were compared to reference values obtained with the random phase approximation. When combining these results with observations of previous benchmarking studies, the rev-vdW-DF2 and PBE-D3 functionals emerge as approaches that should be (relatively) free from a systematic tendency to deliver too negative adsorption energies.

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Section: Models Of Organic Contaminants Zeolites and Adsorption Compl...mentioning

confidence: 99%

Section: Models Of Organic Contaminants Zeolites and Adsorption Compl...mentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Studying the adsorption of emerging organic contaminants in zeolites with dispersion-corrected density functional theory calculations: From numbers to recommendations

Fischer

2022

Preprint

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

Fischer

2023

ChemPhysChem

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The anticonvulsant drug carbamazepine (À ) is an emerging contaminant of considerable concern due to its hazard potential and environmental persistence. 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 maximizes dispersion interactions was identified as the dominant factor determining the interaction strength. Further calculations addressed the role of temperature (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.

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Computational Screening of Hydrophobic Zeolites for the Removal of Emerging Organic Contaminants from Water

Brauer,

Fischer

2024

ChemPhysChem

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The pollution of water resources by pharmaceuticals and agents of personal care products (PPCPs) poses an increasingly pressing issue that has received considerable attention from scientists and government agencies alike. Hydrophobic zeolites can serve as selective adsorbents to remove these contaminants from aqueous solution. So far, the adsorption of PPCPs in zeolites has often been investigated in case studies focusing on a small number of contaminants and one or a few zeolites. We present a computational screening approach to investigate the interaction of 53 PPCPs with 14 all‐silica zeolites, aiming at a more comprehensive understanding of factors that are beneficial for a strong host‐guest interaction and thus an efficient adsorption. The systems are modelled on the classical force field level of theory, allowing for the efficient computational treatment of a large number of PPCP‐zeolite combinations and evaluated in terms of the interaction energy between PPCP and zeolite framework. For selected PPCP‐zeolite combinations additional Free Energy Perturbation simulations are employed to compute Free Energies of Transfer between the aqueous phase and the adsorbed state. These results can serve as a starting point for experimental studies of relevant PPCP‐zeolite combination or more in‐depth theoretical investigations.

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Simulation-based evaluation of zeolite adsorbents for the removal of emerging contaminants

Abstract: Molecular mechanics simulations are used to study the adsorption of organic pollutants in all-silica zeolites.

Cited by 32 publications

References 81 publications

Studying the adsorption of emerging organic contaminants in zeolites with dispersion-corrected density functional theory calculations: From numbers to recommendations

Studying the adsorption of emerging organic contaminants in zeolites with dispersion-corrected density functional theory calculations: From numbers to recommendations

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

Computational Screening of Hydrophobic Zeolites for the Removal of Emerging Organic Contaminants from Water

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