Mussel-Inspired Self-Healing Metallopolymers for Silicon Nanoparticle Anodes

Polymers with supramolecular functionality are receiving increasing attention for rechargeable battery binders as strong supramolecular interactions can facilitate self-healing effects via bond recovery of the cleaved cross-links. Such self-healing capability is useful for emerging high-capacity battery materials that undergo large volume changes. Benchmarking mussel’s sticky byssus cuticle, herein we report a copolymer binder with Fe 3+ –(tris)catechol coordination cross-links, which can induce a self-healing effect for silicon anodes. The high strength of the Fe 3+ –(tris)catechol coordination bond can lead to recovery of the dissociated bond that occurs from the large volume expansion of silicon. The given copolymer also contains monomer units with sufficient flexibility to increase the interchain motions for efficient Fe 3+ –(tris)catechol bond recovery. The superior electrochemical …