100th Anniversary of Macromolecular Science Viewpoint: Solid Polymer Electrolytes in Cathode Electrodes for Lithium...

Solid polymer electrolytes (SPEs) are an important class of ion-transporting materials for enabling safe and high-energy-density all-solid lithium batteries. Within the composite cathode electrode (CCE), an SPE plays a critical role as both binder material for mechanical integrity and electrolyte to facilitate ion transport. The inclusion of an SPE within the CCE leads to the formation of distinctive heterogeneous SPE/solid interfaces that are not present in traditional liquid electrolyte-containing CCE. Here, the viewpoint emphasizes the importance of understanding the interfacial behavior of SPEs in all-solid CCEs. Challenges and opportunities are highlighted in achieving and maintaining good interfacial contact, and the role of interfacial dynamics and nanoconfinement on ion transport. Additionally, routes to achieving high-voltage electrochemical stability through stabilization of interfaces and the development of SPEs with inherently higher oxidative stability are discussed. SPEs with high-voltage stability will provide a pathway to using cathode active materials operating at 4.5 V versus Li/Li⁺ and beyond, which are essential to attaining next-generation higher-energy batteries. Overall, the viewpoint clarifies the importance of targeted research and development of SPEs for enabling all-solid CCEs for lithium batteries.