Computational Evaluation of Mg–Salen Compounds as Subsurface Fluid Tracers: Molecular Dynamics Simulations in Toluene–Water Mixtures and Clay Mineral Nanopores

Greathouse, Jeffery A.; Boyle, Timothy J.; Kemp, Richard A.

doi:10.1021/acs.energyfuels.8b00435

Title: Computational Evaluation of Mg–Salen Compounds as Subsurface Fluid Tracers: Molecular Dynamics Simulations in Toluene–Water Mixtures and Clay Mineral Nanopores

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Abstract

Molecular tracers that can be selectively placed underground and uniquely identified at the surface using simple on-site spectroscopic methods would significantly enhance subsurface fluid monitoring capabilities. To ensure their widespread utility, the solubility of these tracers must be easily tuned to oil- or water-wet conditions as well as reducing or eliminating their propensity to adsorb onto subsurface rock and/or mineral phases. In this work, molecular dynamics simulations were used to investigate the relative solubilities and mineral surface adsorption properties of three candidate tracer compounds comprising Mg–salen derivatives of varying degrees of hydrophilic character. Simulations in water–toluene liquid mixtures indicate that the partitioning of each Mg–salen compound relative to the interface is strongly influenced by the degree of hydrophobicity of the compound. Simulations of these complexes in fluid-filled mineral nanopores containing neutral (kaolinite) and negatively charged (montmorillonite) mineral surfaces reveal that adsorption tendencies depend upon a variety of parameters, including tracer chemical properties, mineral surface type, and solvent type (water or toluene). Simulation snapshots and averaged density profiles reveal insight into the solvation and adsorption mechanisms that control the partitioning of these complexes in mixed liquid phases and nanopore environments. As a result, this work demonstrates the utility of molecular simulationmore »« less

Authors:

Greathouse, Jeffery A. ^[1]; Boyle, Timothy J. ^[1]; Kemp, Richard A. ^[1]; Univ. of New Mexico, Albuquerque, NM ^[2]

Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
(United States)

Publication Date:: 2018-04-11

Research Org.:: Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Sponsoring Org.:: USDOE National Nuclear Security Administration (NNSA)

OSTI Identifier:: 1444086

Report Number(s):: SAND-2018-3643J
Journal ID: ISSN 0887-0624; 663974

Grant/Contract Number:: AC04-94AL85000

Resource Type:: Accepted Manuscript

Journal Name:: Energy and Fuels

Additional Journal Information:: Journal Volume: 32; Journal Issue: 4; Journal ID: ISSN 0887-0624

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Greathouse, Jeffery A., Boyle, Timothy J., Kemp, Richard A., and Univ. of New Mexico, Albuquerque, NM. Computational Evaluation of Mg–Salen Compounds as Subsurface Fluid Tracers: Molecular Dynamics Simulations in Toluene–Water Mixtures and Clay Mineral Nanopores.  United States: N. p., 2018. 
Web.  doi:10.1021/acs.energyfuels.8b00435.

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                    Greathouse, Jeffery A., Boyle, Timothy J., Kemp, Richard A., & Univ. of New Mexico, Albuquerque, NM. Computational Evaluation of Mg–Salen Compounds as Subsurface Fluid Tracers: Molecular Dynamics Simulations in Toluene–Water Mixtures and Clay Mineral Nanopores.  United States.  https://doi.org/10.1021/acs.energyfuels.8b00435

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                    Greathouse, Jeffery A., Boyle, Timothy J., Kemp, Richard A., and Univ. of New Mexico, Albuquerque, NM. Wed .  
"Computational Evaluation of Mg–Salen Compounds as Subsurface Fluid Tracers: Molecular Dynamics Simulations in Toluene–Water Mixtures and Clay Mineral Nanopores".  United States.  https://doi.org/10.1021/acs.energyfuels.8b00435.  https://www.osti.gov/servlets/purl/1444086.

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@article{osti_1444086,

  title        = {Computational Evaluation of Mg–Salen Compounds as Subsurface Fluid Tracers: Molecular Dynamics Simulations in Toluene–Water Mixtures and Clay Mineral Nanopores},

  author       = {Greathouse, Jeffery A. and Boyle, Timothy J. and Kemp, Richard A. and Univ. of New Mexico, Albuquerque, NM},

  abstractNote = {Molecular tracers that can be selectively placed underground and uniquely identified at the surface using simple on-site spectroscopic methods would significantly enhance subsurface fluid monitoring capabilities. To ensure their widespread utility, the solubility of these tracers must be easily tuned to oil- or water-wet conditions as well as reducing or eliminating their propensity to adsorb onto subsurface rock and/or mineral phases. In this work, molecular dynamics simulations were used to investigate the relative solubilities and mineral surface adsorption properties of three candidate tracer compounds comprising Mg–salen derivatives of varying degrees of hydrophilic character. Simulations in water–toluene liquid mixtures indicate that the partitioning of each Mg–salen compound relative to the interface is strongly influenced by the degree of hydrophobicity of the compound. Simulations of these complexes in fluid-filled mineral nanopores containing neutral (kaolinite) and negatively charged (montmorillonite) mineral surfaces reveal that adsorption tendencies depend upon a variety of parameters, including tracer chemical properties, mineral surface type, and solvent type (water or toluene). Simulation snapshots and averaged density profiles reveal insight into the solvation and adsorption mechanisms that control the partitioning of these complexes in mixed liquid phases and nanopore environments. As a result, this work demonstrates the utility of molecular simulation in the design and screening of molecular tracers for use in subsurface applications.},

  doi          = {10.1021/acs.energyfuels.8b00435},

  journal      = {Energy and Fuels},

  number       = 4,

  volume       = 32,

  place        = {United States},

  year         = {2018},

  month        = {4}

}

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