This perspective reviews current strategies to decouple segmental motion and ionic conductivity for lithium polymer battery electrolytes, including an outlook for potential future improvements.

Organic materials derived from biomass can constitute a viable option as replacements for inorganic materials in lithium-ion battery electrodes owing to their low production costs, recyclability, and structural diversity. Among them, conjugated carbonyls have become the most promising type of organic electrode material as they present high theoretical capacity, fast reaction kinetics, and quasi-infinite structural diversity. In this letter, we report a new perylene-based all-organic redox battery comprising two aromatic conjugated carbonyl electrode materials, the prelithiated tetra-lithium perylene-3,4,9,10-tetracarboxylate (PTCLi6) as negative electrode material and the poly(N-n-hexyl-3,4,9,10-perylene tetracarboxylic)imide (PTCI) as positive electrode material. The resulting battery shows promising long-term cycling stability up to 200 cycles. In view of the enhanced cycling performances, the two organic materials studied herein are proposed as suitable candidates for the development of new all-organic lithium-ion batteries.

Polymerized ionic liquids (poly­(ILs)) are considered highly promising for the realization of high-performance and intrinsically safer electrolytes for rechargeable batteries due to their high charge density. However, to date little is known about the ion conduction mechanism for this class of solid polymer electrolytes (SPEs). Herein, we performed an in-depth characterization of a homologous series of 1-alkyl-3-vinylimidazolium bis­(trifluoro­methane)­sulfonimide-derived homopolymers, i.e., p­(C n VIm-TSI) with n = 2, 4, 6, 8, and 10, serving as a model compound family. A particular focus was set on the interplay of the physicochemical properties, nanostructure, and ionic conductivity as well as on the impact of the additional incorporation of a lithium salt, LiTFSI. The results reveal that the nanostructure of these self-assembling poly­(ILs) plays a decisive role for the ion conduction mechanism, allowing for a (partial) decoupling of charge transport and segmental relaxation of the polymer backbone.