Ion Transport in the EMITFSI/PVDF System at Different Temperatures: A Molecular Dynamics Simulation

MH Qu and SS Li and J Chen and YQ Xiao and JJ Xiao, ACS OMEGA, 7, 9333-9342 (2022).

DOI: 10.1021/acsomega.1c06160

We used all-atom molecular dynamics simulations to study the ion transport in the 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide/poly(vinylidene fluoride) (EMITFSI/PVDF) system with 40.05 wt % EMITFSI at different temperatures. The glass-transition temperature (T-g = 204 K) of this system shows a good agreement with the experimental value (200 K). With the increase of temperature, the peaks of the pair correlation function show an increasing trend. Interestingly, the coordination numbers of ion pairs and the degree of independent ion motion are mainly affected by the binding energy between ion pairs as the temperature increases. In addition, the ion transport properties with increasing temperature can be studied by the ion-pair relaxation times, ion-pair lifetimes, and diffusion coefficients. The simulation results illustrate that the ion transport is intensified. Especially, the cations can always diffuse faster than the anions. The power law shows that mobilities of anions and cations are seen to exhibit a "superionic" behavior. With the increase of temperature, transference numbers of anions decrease first and then increase and transference numbers of cations show the opposite changes; ionic conductivity increases gradually; and viscosity decreases gradually, indicating that the diffusion resistance of ions decreases. In general, after adding PVDF into the EMITFSI system, the glass- transition temperature and viscosity increase, the ionic conductivity and degree of independent ion motion decrease, and diffusion coefficients of cations decrease faster than those of the anions.

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