Polymerized ionic liquids (polyILs) are a novel class of functional polymers that combine the unique physicochemical properties of molecular ionic liquids (e.g. wide electrochemical windows, negligible vapor pressures, and ionic conduction) with the outstanding mechanical characteristics of polymers. These materials are promising for a variety of applications including dye-sensitized solar cells, portable batteries, actuators, field-effect transistors, and electrochromic devices. However, the ionic conductivity of polyILs, which is one of the most critical properties in the context of electrochemical energy applications, drops by many orders of magnitude in comparison to their low molecular weight counterparts upon polymerization. Since in polyILs one type of ion is covalently tethered onto the polymer matrix, only the counter-ions move freely thereby contributing to long-range charge transport. Thus, the possibility to select the faster counter-ions <i>a priori</i> is particularly attractive for this class of polymer electrolytes. However, many electrochemical energy devices require ionic conductivities above 1 mS/cm for efficient operation but the state-of-the-art neat polyILs remain orders of magnitude below this value at ambient conditions. In this talk, I will focus on current strategies to develop new polyILs with high ionic conductivity for different electrochemical energy technologies. Unlike the standard poly(ethylene oxide)-based electrolytes, detailed analysis reveals strong decoupling between ionic conduction and segmental dynamics in PolyILs, implying the inadequacy of the classical theories of electrolytes, in contrast to their low molecular weight counterparts. Some new insights into the dominant mechanisms of charge transport and dynamics obtained from combined experimental and theoretical efforts will be presented.

Ion transport and dynamics in polymerized ionic liquids: Insights from broadband dielectric spectroscopy

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ACS Fall 2022

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