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Theoretical study of adsorption of nitrogen-containing environmental contaminants on kaolinite surfaces

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Abstract

The adsorption of nitrogen-containing compounds (NCCs) including 2,4,6-trinitrotoluene (TNT), 2,4-dinitrotoluene (DNT), 2,4-dinitroanisole (DNAN), and 3-nitro-1,2,4-triazol-5-one (NTO) on kaolinite surfaces was investigated. The M06-2X and M06-2X-D3 density functionals were applied with the cluster approximation. Several different positions of NCCs relative to the adsorption sites of kaolinite were examined, including NCCs in perpendicular and parallel orientation toward both surface models of kaolinite. The binding between the target molecules and kaolinite surfaces was analyzed and bond energies were calculated applying the atoms in molecules (AIM) method. All NCCs were found to prefer a parallel orientation toward both kaolinite surfaces, and were bound more strongly to the octahedral than to the tetrahedral site. TNT exhibited the strongest interaction with the octahedral surface and DNAN with the tetrahedral surface of kaolinite. Hydrogen bonding was shown to be the dominant non-covalent interaction for NCCs interacting with the octahedral surface of kaolinite with a small stabilizing effect of dispersion interactions. In the case of adsorption on the tetrahedral surface, kaolonite–NCC binding was shown to be governed by the balance between hydrogen bonds and dispersion forces. The presence of water as a solvent leads to a significant decrease in the adsorption strength for all studied NCCs interacting with both kaolinite surfaces.

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Acknowledgments

This work was facilitated by support from the High Performance Computing Major Shared Resource Center at the Engineer Research and Development Center (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 US 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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Authors and Affiliations

  1. US Army Engineer Research and Development Center (ERDC), Vicksburg, MS, 39180, USA

    Andrea Michalkova Scott & Frances C. Hill

  2. Badger Technical Services, LLC, Vicksburg, MS, 39180, USA

    Elizabeth A. Burns

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  1. Andrea Michalkova Scott
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  2. Elizabeth A. Burns
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  3. Frances C. Hill
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Correspondence to Andrea Michalkova Scott.

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Scott, A.M., Burns, E.A. & Hill, F.C. Theoretical study of adsorption of nitrogen-containing environmental contaminants on kaolinite surfaces. J Mol Model 20, 2373 (2014). https://doi.org/10.1007/s00894-014-2373-7

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