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Measurement of the Potential Rates of Dissimilatory Nitrate Reduction to Ammonium Based on 14NH4+/15NH4+ Analyses via Sequential Conversion to N2O
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Coupled jump rotational dynamics in aqueous nitrate solutions.

Puja Banerjee1, Subramanian Yashonath1, Biman Bagchi1

  • 1Solid State and Structural Chemistry Unit, Indian Institute of Science, Bangalore 560012, India.

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|December 18, 2016
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Nitrate ions in water exhibit large rotational jumps, driven by water molecule hydrogen bond rearrangements. Two distinct mechanisms were identified, influencing nitrate ion rotation and solvent dynamics.

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Area of Science:

  • Physical Chemistry
  • Computational Chemistry
  • Solution Chemistry

Background:

  • Nitrate ions (NO3-) possess unique trigonal planar geometry and charge distribution.
  • Water's extensive hydrogen bond network influences solute dynamics.
  • Coupling between solute rotation and solvent rearrangement is crucial in aqueous solutions.

Purpose of the Study:

  • To investigate the dynamical characteristics of nitrate ions in aqueous solutions.
  • To elucidate the mechanisms of hydrogen bond rearrangement in water around nitrate ions.
  • To understand the coupling between nitrate ion reorientation and water dynamics.

Main Methods:

  • Detailed atomistic simulations
  • Theoretical analyses
  • Calculation of torque on nitrate ion
  • Computation of time correlation functions

Main Results:

  • Nitrate ions exhibit large amplitude rotational jump motions coupled to water hydrogen bond dynamics.
  • Two distinct hydrogen bond exchange mechanisms in water were identified, promoting nitrate ion jumps.
  • Different reorientational behaviors (out-of-plane vs. in-plane) of nitrate ions were observed for each mechanism.
  • Coupled reorientational jump dynamics and relaxation times for nitrate and water were computed.

Conclusions:

  • The study reveals intricate coupling between nitrate ion rotational jumps and water hydrogen bond network rearrangements.
  • Two mechanisms of hydrogen bond exchange significantly influence the nature and magnitude of nitrate ion reorientation.
  • Findings provide insights into the solute-solvent dynamics in aqueous nitrate solutions.