Understanding the
mechanisms controlling ionic conductivity is
critical for the development of the next generation of batteries and
supercapacitors. This paper discusses the significant role played
by ionic correlations in conductivity of concentrated ionic systems.
Our studies of an organic ionic plastic crystal reveal that correlations
in ions dynamics suppress conductivity by 25–100 times in comparison
to the expected uncorrelated ionic conductivity estimated from the
Nernst–Einstein relationship. Additional analysis also demonstrates
that ionic correlations suppress conductivity in polymerized ionic
liquids and gel by ∼10 times. Thus, ionic correlations, usually
neglected in many studies, play a very important role in conductivity
of concentrated ionic systems. These results cannot be explained by
a diffusion of ion pairs because all these systems are essentially
single ion conductors. In contrast, strongly correlated motions of
mobile ions with the same charge (cation–cation or anion–anion
correlations) are the major mechanism suppressing the ionic conductivity
in these systems. On the basis of these results, we emphasize that
charge transport rather than ion diffusion is critical for electrolyte
performance and suggest the potential design of plastic crystals and
polymer electrolytes with enhanced ionic conductivity.
Organic ionic plastic crystals (OIPCs) are promising solid electrolytes because of their inherent advantages such as non-volatility, non-flammability, good thermal stability, favourable plasticity, and improved electrolyte/electrode interfacial contact. Incorporating nanoparticles...
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