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We developed a hydrodynamic theory for ion diffusion, showing hydrodynamic interactions universally dictate ion correlations in electrolytes and ionic liquids. Conductivity contributions arise from local structure and subdiffusive relaxation, not just ideal fluid flow.

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Area of Science:

  • Physical Chemistry
  • Computational Chemistry
  • Theoretical Chemistry

Background:

  • Hydrodynamic interactions are crucial for understanding ion diffusion in electrolytes and ionic liquids.
  • Previous work focused on self-diffusion, necessitating a generalized theory for pair diffusion.
  • Correlated ion motion influences macroscopic transport properties like conductivity.

Purpose of the Study:

  • To present a generalized hydrodynamic theory for pair diffusion in systems with periodic boundary conditions.
  • To compare theoretical predictions with Molecular Dynamics simulations for electrolytes and ionic liquids.
  • To elucidate the role of hydrodynamic interactions and other factors in determining ionic conductivity.

Main Methods:

  • Developed a hydrodynamic theory for pair diffusion with periodic boundary conditions.
  • Performed Molecular Dynamics simulations of a liquid carbonate electrolyte and two ionic liquids.
  • Analyzed correlated ion motion and conductivity contributions.

Main Results:

  • The theory shows good agreement with simulation data, confirming universal hydrodynamic control of ion correlations.
  • Hydrodynamic interactions between ions of like and unlike charges largely cancel in total conductivity calculations.
  • Significant conductivity contributions originate from deviations from ideal fluid flow, including local structure and subdiffusive relaxation.
  • Momentum conservation is vital for ionic liquids, influenced by ionic masses.

Conclusions:

  • Hydrodynamic theory provides a robust framework for describing pair diffusion and ion correlations.
  • Ionic conductivity is primarily determined by non-ideal fluid behavior and dynamic processes.
  • The developed formalism can aid in estimating finite-size effects on conductivity and diffusion coefficients.