Flexible aqueous zinc-ion batteries (ZIBs) are promising candidates for next-generation wearable electronics and soft robotics, yet their development is hindered by the non-selective ion transport of conventional hydrogel electrolytes, which induces concentration polarization, uneven Zn 2+ flux, and dendrite formation, ultimately causing battery failure. Here, a microphase-separated single-zinc-ion conducting hydrogel electrolyte (SIHE) constructed via polymer chain disentanglement within a polyanionic zinc-alginate (ZA) matrix is reported. Due to the pronounced steric disparity between Zn 2+ and the alginate chains, ZA holds intrinsic potential for ion-selective transport. However, spontaneous chain entanglement within the alginate network under the applied electric field severely impedes the formation of continuous ion transport pathways, limiting Zn 2+ conduction. By incorporating Nafion, well-defined hydrophilic/hydrophobic domains are induced that simultaneously relax the entangled polymer network and establish continuous Zn 2+ -conducting pathways. This microstructural engineering enables a high Zn 2+ transference number of 0.967 and ionic conductivity of 25.5 mS cm −1 , resolving the long-standing trade-off between ion selectivity and transport kinetics. The zinc-alginate/Nafion (ZA/N) electrolyte enables dendrite-free cycling for over 4600 h. The ZA/N-based flexible ZIB retains 90% capacity after 5000 cycles at 10 A g −1 . This work presents a general strategy to engineer high-performance SIHEs for safe and durable flexible zinc-ion batteries.
Functional separator which facilitates the fast transport of Li + but obstructs the permeation of polysulfides is highly required for durable lithium-sulfur (Li-S) batteries. Here, we report a facile approach to developing such functional separator by coating the commercial polypropylene separator with a unique solution-processable polymer featuring both intrinsic microporosity and ion-selective functionality. The polymer is designed with contorted and rigid backbones, which incorporates zwitterionic side chains with both sulfophilic and lithiophilic groups, to produce confined ionic channels for selective ion transport via the chemical interactions with lithium polysulfides. Therefore, when used in the cell configuration, the as-developed functional separator can not only allow the fast Li + conduction but also obstruct the penetration of bulky polysulfides, thus resulting in obvious shuttle suppression as well as the resultant credible and stable sulfur electrochemistry . Thanks to these advantages, the Li-S batteries implementing the as-developed functional separator possess high cycling ability and decent rate performance.
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