Mussel‐Inspired Polymer Binders for Organic Electrodes

Abstract The development of polymer binders is necessary to meet the growing demands of modern energy storage technologies. While catechol‐containing materials are proven successful in silicon anodes, their application in organic batteries remains unexplored. In this contribution, the synthesis of four polymers are described with nearly identical side chain composition but varying backbone structures. The materials are used to investigate the effect of polymer backbone structure on the binding abilities of catechol‐containing materials. Comparative analysis with the commonly used polyvinylidene fluoride (PVDF) binder aims to address two critical questions: 1) Can catechol‐rich polymers replace PVDF for use in organic cathodes? and 2) Does the choice of polymer backbone affect the performance of the battery?. The investigation reveals that supramolecular interactions, such as π–π stacking and coordination bonding, are pivotal features of catechol binders. Among the catechol‐rich polymers, the polyacrylate binder stands out, likely attributed to its high flexibility. Additionally, introducing an oxygen atom into a catechol‐rich polynorbornene enhances lithium‐ion conductivity and rate performance. Overall, the findings highlight the viability of catechol‐containing polymers as organic cathode binders, and that the choice of polymer backbone is a crucial factor for their use as lithium‐ion battery binder materials.