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Thermodynamically Consistent Force Field for Coarse-Grained Modeling of Aqueous Electrolyte Solution.

Carlos Nieto-Draghi1, Bernard Rousseau2

  • 1IFP Energies nouvelles , 1-4 Avenue de Bois Préau , 92852 Rueil-Malmaison , France.

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|February 21, 2019
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Summary

We developed a new method to simulate charged particles using dissipative particle dynamics (DPD). This approach accurately predicts ion behavior in solutions, improving molecular simulations for electrolytes.

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Area of Science:

  • Computational chemistry
  • Physical chemistry
  • Soft matter physics

Background:

  • Dissipative Particle Dynamics (DPD) is a mesoscopic simulation technique.
  • Accurate parameterization of inter-particle interactions is crucial for DPD.
  • Modeling charged particles in solution presents significant challenges.

Purpose of the Study:

  • To develop a thermodynamically consistent methodology for parameterizing charged particle interactions within the DPD framework.
  • To optimize DPD interaction parameters using experimental osmotic pressure data for ionic solutions.
  • To establish a predictive method for ion-water and ion-ion interactions in DPD.

Main Methods:

  • Utilized experimental osmotic pressure data as a function of salinity for parameter optimization.
  • Determined DPD repulsion parameters (Na+-water, Cl--water, Na+-Cl-) using osmotic and activity coefficients.
  • Proposed a linear relationship between ion hydration-free energies and ion-water repulsion parameters.
  • Employed two strategies for anion-cation interaction parameterization: numerical optimization and a predictive approach based on hydration energies.

Main Results:

  • Successfully parameterized DPD interactions for NaCl aqueous solutions.
  • Achieved mean average deviations <4% for osmotic pressure data using numerical optimization.
  • Developed a predictive approach with a mean absolute relative deviation of ~13% for anion-cation interactions, outperforming previous methods.
  • Demonstrated a linear correlation between ion hydration-free energies and ion-water repulsion parameters for halide and alkaline ions.

Conclusions:

  • The proposed methodology provides a thermodynamically consistent way to parameterize charged particle interactions in DPD.
  • The optimized DPD parameters accurately reproduce experimental osmotic pressure data for electrolyte solutions.
  • The predictive approach based on hydration energies offers a promising route for parameterizing interactions involving a wider range of ions.
  • This work enhances the capability of DPD for simulating complex ionic systems.