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Electrolytes based on organic solvents used in current Li-ion batteries are not compatible with the next-generation energy storage technologies including those based on Li metal. Thus, there has been an increase in research activities investigating solid-state electrolytes, ionic liquids (ILs), polymers, and combinations of these. This Account will discuss some of the work from our teams in these areas. Similarly, other metal-based technologies including Na, Mg, Zn, and Al, for example, are being considered as alternatives to Li-based energy storage. However, the materials research required to effectively enable these alkali metal based energy storage applications is still in its relative infancy. Once again, electrolytes play a significant role in enabling these devices, and research has for the most part progressed along similar lines to that in advanced lithium technologies. Some of our recent contributions in these areas will also be discussed, along with our perspective on future directions in this field. For example, one approach has been to develop single-ion conductors, where the anion is tethered to the polymer backbone, and the dominant charge conductor is the lithium or sodium countercation. Typically, these present with low conductivity, whereas by using a copolymer approach or incorporating bulky quaternary ammonium co-cations, the effective charge separation is increased thus leading to higher conductivities and greater mobility of the alkali metal cation. This has been demonstrated both experimentally and via computer simulations. Further enhancements in ion transport may be possible in the future by designing and tethering more weakly associating anions to the polymer backbone. The second approach considers ion gels or composite polymer electrolytes where a polymerized ionic liquid is the matrix that provides both mechanical robustness and ion conducting pathways. The block copolymer approach is also demonstrated, in this case, to simultaneously provide mechanical properties and high ionic conductivity when used in combination with ionic-liquid electrolytes. The ultimate electrolyte material that will enable all high-performance solid-state batteries will have ion transport decoupled from the mechanical properties. While inorganic conductors can achieve this, their rigid, brittle nature creates difficulties. On the other hand, ionic polymers and their composites provide a rich area of chemistry to design and tune high ionic conductivity together with ideal mechanical properties.

Innovative Electrolytes Based on Ionic Liquids and Polymers for Next-Generation Solid-State Batteries