Lithium–sulfur (Li–S)
batteries are widely regarded
as one of the most promising next-generation energy storage devices
due to their high energy density. Nevertheless, fast capacity fade
caused by the tremendous volume changes of S-based cathodes and polysulfide
shuttling during cycling remains to be effectively tackled prior to
practical applications. Inspired by skeletal muscle, here, we develop
a responsive network/confinement network blend (RCB) binder to remove
the above bottlenecks. The as-developed binder is prepared through
simply blending an aqueous hyaluronic acid (HA) solution and an oily
solution with a tetrazole group-based copolymer of polyacrylonitrile
and poly(ethylene glycol) bisazide. Hydrophobic tetrazole group-containing
polymer (denoted as PCP) condenses in the mixture solution forming
submicrometer-sized irregular spherical domains as the confinement
network similar to myofilament, while water-soluble HA constructs
a responsive network mimicking the fascia of skeletal muscle; meanwhile,
the formed responsive network can coordinate the force among the confinement
network by linking with PCP via ionic bonding. The RCB binder exhibits
superior mechanical matching and adhesive properties and thus can
effectively accommodate the huge volume change of S-based electrodes.
Additionally, abundant polar groups such as carboxylic, amide, cyano,
and tetrazole groups allow the RCB binder to effectively capture lithium
polysulfide through strong anchoring effect. As a result, Li–S
batteries assembled with a limited RCB binder dosage (5 wt % of the
whole electrode film weight) exhibit remarkable improvement in both
cycling and rate performance, even under high S loadings. Such skeletal
muscle-inspired binder design helps boost the advance of S-based cathode
binders toward practical battery applications.