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Polymer electrolytes are essential elements of current and next-generation energy storage applications. An important class of polymer electrolytes is ionomers, in which one of the ions is covalently bound to the polymer backbone. Ionomers are currently used in fuel cells, and show extraordinary promise as solid electrolytes in batteries for transportation and portablepower applications. Solid electrolytes are desirable for a variety of reasons. A primary one is safety: the lack of solvent leads to fewer electrochemical reactions (e.g. with the electrodes) and the absence of flammable liquids. Solvent-free electrolytes allow for less packaging (and hence higher energy density batteries) and easier manufacture. Single-ion conductors such as ionomers also have the advantage of higher efficiency (high lithium transference numbers), since the anions are bound to the polymer backbone and the current is primarily due to the cations that actively participate in the electrochemical reactions. However, to date ionomeric materials do not have sufficiently high conductivities. Ion transport mechanisms in ionomers and their relation to molecular structure are poorly understood, although it is known that ion transport is coupled to polymeric motion and to the nanoscale morphology of ionic aggregates that often self-assemble in the polymer matrix. In this project we investigate the morphology and ion dynamics in ionomer melts using ab initio calculations, NMR experiments, and both atomistic and coarse-grained molecular dynamics simulations. We find that the aggregate morphology depends strongly on polymer architecture, neutralizing cation, and degree of neutralization. This morphology in turn affects the counterion dynamics; we find that counterions diffuse more quickly in systems with percolated aggregates than in systems with discrete aggregates.

Effects of morphology on ion transport in ionomers for energy storage.