Issue 20, 2024

Incorporating solvent effects in DFT: insights from cation exchange in faujasites

Abstract

Zeolites are versatile materials renowned for their extra-framework cation exchange capabilities, with applications spanning diverse fields, including nuclear waste treatment. While detailed experimental characterization offers valuable insight, density functional theory (DFT) proves particularly adept at investigating ion exchange in zeolites, owing to its atomic and electronic resolution. However, the prevalent occurrence of zeolitic ion exchange in aqueous environments poses a challenge to conventional DFT modeling, traditionally conducted in a vacuum. This study seeks to enhance zeolite modeling by systematically evaluating predictive differences across varying degrees of aqueous solvent inclusion. Specifically focusing on monovalent cation exchange in Na-X zeolites, we explore diverse modeling approaches. These range from simple dehydrated systems (representing bare reference states in vacuum) to more sophisticated models that incorporate aqueous solvent effects through explicit water molecules and/or a dielectric medium. Through comparative analysis of DFT and semi-empirical DFT approaches, along with their validation against experimental results, our findings underscore the necessity to concurrently consider explicit and implicit solvent effects for accurate prediction of zeolitic ionic exchange.

Graphical abstract: Incorporating solvent effects in DFT: insights from cation exchange in faujasites

Supplementary files

Article information

Article type
Paper
Submitted
31 Janv. 2024
Accepted
01 Maijs 2024
First published
02 Maijs 2024
This article is Open Access
Creative Commons BY-NC license

Phys. Chem. Chem. Phys., 2024,26, 14561-14572

Incorporating solvent effects in DFT: insights from cation exchange in faujasites

A. T. Ta, A. Daouli, R. S. Ullberg, E. Fonseca, V. Proust, A. Grandjean, R. G. Hennig, H. zur Loye, M. Badawi and S. R. Phillpot, Phys. Chem. Chem. Phys., 2024, 26, 14561 DOI: 10.1039/D4CP00467A

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