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Theoretical predictions of thermodynamic parameters of adsorption of nitrogen containing environmental contaminants on kaolinite

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Abstract

In this study thermodynamic parameters of adsorption of nitrogen containing environmental contaminants (NCCs, 2,4,6, trinitrotoluene (TNT), 2,4-dinitrotoluene (DNT), 2,4-dinitroanisole (DNAN), and 3-one-1,2,4-triazol-5-one (NTO)) interacting with the tetrahedral and octahedral surfaces of kaolinite were predicted. Adsorption complexes were investigated using a density functional theory and both periodic and cluster approach. The complexes, modeled using the periodic boundary conditions approach, were fully optimized at the BLYP-D2 level to obtain the structures and adsorption energies. The relaxed kaolinite-NCCs structures were used to prepare cluster models to calculate thermodynamic parameters and partition coefficients at the M06-2X-D3 and BLYP-D2 levels from the gas phase. The entropy effect on the Gibbs free energies of adsorption of NCCS on kaolinite was also studied and compared with available experimental data. The results showed that in all calculated models, the NCCs molecules are physisorbed and they favor a parallel orientation toward both kaolinite surfaces. It was found that all calculated NCCs compounds are more stable on the octahedral than on the tetrahedral surface of kaolinite. The Gibbs free energies and partition coefficients were also predicted for interactions of NCCs with Na-kaolinite from aqueous solution. Calculations revealed adsorption of NCCs is effective from the gas phase on both cation free kaolinite surfaces and on Na-kaolinite from aqueous solution at room temperature. Theoretical data were validated against experimental results, and the reasons for small differences between calculated and measured partition coefficients are discussed.

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Acknowledgments

This work was facilitated by support from the High Performance Computing Distributed Shared Resource Center at the ERDC (Vicksburg, MS). The use of trade, product, or firm names in this report is for descriptive purposes only and does not imply endorsement by the U.S. Government. Results in this study were funded and obtained from research conducted under the Environmental Quality Technology Program of the United States Army Corps of Engineers by the US Army ERDC. Permission was granted by the Chief of Engineers to publish this information. The findings of this report are not to be construed as an official Department of the Army position unless so designated by other authorized documents.

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  1. U. S. Army Engineer Research and Development Center (ERDC), 3909 Halls Ferry Rd., Vicksburg, MS, 39180, USA

    Andrea Michalkova Scott, Brandon J. Lafferty & Frances C. Hill

  2. Badger Technical Services, LLC, 3909 Halls Ferry Rd., Vicksburg, MS, 39180, USA

    Elizabeth A. Burns

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  1. Andrea Michalkova Scott
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Scott, A.M., Burns, E.A., Lafferty, B.J. et al. Theoretical predictions of thermodynamic parameters of adsorption of nitrogen containing environmental contaminants on kaolinite. J Mol Model 21, 21 (2015). https://doi.org/10.1007/s00894-015-2577-5

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