4.8 Article

Electric-Field-Induced Spatially Dynamic Heterogeneity of Solvent Motion and Cation Transference in Electrolytes

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PHYSICAL REVIEW LETTERS
卷 128, 期 19, 页码 -

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AMER PHYSICAL SOC
DOI: 10.1103/PhysRevLett.128.198002

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  1. U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES)

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The study found that electric fields primarily result in migration of charged species in electrolytic solutions, and different solvation motifs and concentrations can affect the cation transference number. At a certain concentration, the dynamic heterogeneity of solvent molecules is minimized and the transference number approaches zero.
While electric fields primarily result in migration of charged species in electrolytic solutions, the solutions are dynamically heterogeneous. Solvent molecules within the solvation shells of the cation will be dragged by the field while free solvent molecules will not. We combine electrophoretic NMR measurements of ion and solvent velocities under applied electric fields with molecular dynamics simulations to interrogate different solvation motifs in a model liquid electrolyte. Measured values of the cation transference number (t0??) agree quantitatively with simulation-based predictions over a range of electrolyte concentrations. Solvent-cation interactions strongly influence the concentration-dependent behavior of t0??. We identify a critical concentration at which most of the solvent molecules lie within solvation shells of the cations. The dynamic heterogeneity of solvent molecules is minimized at this concentration where t0?? is approximately equal to zero.

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