NO3- Coordination in Aqueous Solutions by 15N/14N and 18O/natO Isotopic Substitution: What Can We Learn from Molecular Simulation?

Chialvo, Ariel A.; Vlcek, Lukas

doi:10.1021/jp510355u

Title: NO3- Coordination in Aqueous Solutions by ¹⁵N/¹⁴N and 18O/natO Isotopic Substitution: What Can We Learn from Molecular Simulation?

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Abstract

We explore the deconvolution of the water-nitrate correlations by the first-order difference approach involving neutron diffraction of heavy- and null-aqueous solutions of KNO₃ under ¹⁴N ¹⁵N and natON ¹⁸ON substitutions to achieve a full characterization of the first water coordination around the nitrate ion. For that purpose we performed isobaric-isothermal simulations of 3.5m KNO₃ aqueous solutions at ambient conditions to generate the relevant radial distribution functions (RDF) required in the analysis (a) to identify the individual partial contributions to the total neutron weighted distribution function, (b) to isolate and assess the contribution of NO₃ -!K⁺ pair formation, (c) to test the accuracy of the NDIS-based coordination calculations and XRDbased assumptions, and (d) to describe the water coordination around both the nitrogen and oxygen sites of the nitrate ion.

Authors:

Chialvo, Ariel A. ^[1]; Vlcek, Lukas ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Publication Date:: Tue Dec 16 00:00:00 EST 2014

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Science (SC)

OSTI Identifier:: 1185735

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry

Additional Journal Information:: Journal Volume: 119; Journal Issue: 2; Journal ID: ISSN 1520-6106

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; nitrate ion hydration; 14N 15N and natON 18ON isotopic substitution; NDIS, XRD; molecular dynamics; coordination numbers

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                    Chialvo, Ariel A., and Vlcek, Lukas. NO3- Coordination in Aqueous Solutions by 15N/14N and 18O/natO Isotopic Substitution: What Can We Learn from Molecular Simulation?.  United States: N. p., 2014. 
Web.  doi:10.1021/jp510355u.

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                    Chialvo, Ariel A., & Vlcek, Lukas. NO3- Coordination in Aqueous Solutions by 15N/14N and 18O/natO Isotopic Substitution: What Can We Learn from Molecular Simulation?.  United States.  https://doi.org/10.1021/jp510355u

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                    Chialvo, Ariel A., and Vlcek, Lukas. Tue .  
"NO3- Coordination in Aqueous Solutions by 15N/14N and 18O/natO Isotopic Substitution: What Can We Learn from Molecular Simulation?".  United States.  https://doi.org/10.1021/jp510355u.  https://www.osti.gov/servlets/purl/1185735.

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@article{osti_1185735,

  title        = {NO3- Coordination in Aqueous Solutions by 15N/14N and 18O/natO Isotopic Substitution: What Can We Learn from Molecular Simulation?},

  author       = {Chialvo, Ariel A. and Vlcek, Lukas},

  abstractNote = {We explore the deconvolution of the water-nitrate correlations by the first-order difference approach involving neutron diffraction of heavy- and null-aqueous solutions of KNO3 under 14N 15N and natON 18ON substitutions to achieve a full characterization of the first water coordination around the nitrate ion. For that purpose we performed isobaric-isothermal simulations of 3.5m KNO3 aqueous solutions at ambient conditions to generate the relevant radial distribution functions (RDF) required in the analysis (a) to identify the individual partial contributions to the total neutron weighted distribution function, (b) to isolate and assess the contribution of NO3 -!K+ pair formation, (c) to test the accuracy of the NDIS-based coordination calculations and XRDbased assumptions, and (d) to describe the water coordination around both the nitrogen and oxygen sites of the nitrate ion.},

  doi          = {10.1021/jp510355u},

  journal      = {Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry},

  number       = 2,

  volume       = 119,

  place        = {United States},

  year         = {Tue Dec 16 00:00:00 EST 2014},

  month        = {Tue Dec 16 00:00:00 EST 2014}

}

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Title: NO3- Coordination in Aqueous Solutions by 15N/14N and 18O/natO Isotopic Substitution: What Can We Learn from Molecular Simulation?

Abstract

Citation Formats

Title: NO3- Coordination in Aqueous Solutions by ¹⁵N/¹⁴N and 18O/natO Isotopic Substitution: What Can We Learn from Molecular Simulation?