Polymers bearing pendant catechols for organic electrode-active materials in lithium-ion batteries

Herein, we describe the synthesis and organometallic-mediated radical polymerization of 1-vinyl-3-alkylimidazolium-type monomers bearing pendant catechols in its protected version, using a presynthesized alkyl‒cobalt(III) complex as monocomponent initiator/mediating agent in a controlled fashion. A neat post-polymerization deprotection, followed by facile anion exchange reactions afforded a novel multi-functional poly(ionic liquids)-bearing free catechol functionalities. Prototype Lithium-ion battery, consisting a binder- and current collector-free electroactive polymer-supported buckypaper as the composite cathode, delivered an impressive specific capacity in the range of 199–230 mA h g‒1, relatively at high discharge potential = 3.2–3.4 V (vs Li/Li+), as calculated from CV and galvanostatic charge-discharge experiments. The superior electrochemical performance of the composite cathode consisting of PIL-catechols active-material, in comparison with poly(dopaminde acrylamide) is ascribed to the intrinsic Li-ion conductivity and enhanced surface activity of the imidazolium backbone with TFSI counteranion, compared to the acrylamide backbone.