https://doi.org/10.1002/slct.202507548

In this work, we designed an intrinsic self-healing hydrogel polymer electrolyte (HGPE) through a synergistic strategy that combines hydrogen bonding, dynamic covalent chemistry, and noncovalent interactions. The Zn2+ ion-induced network densification has created a non-porous, highly cross-linked hydrogel matrix with superior tensile properties, ionic conductivity, cation transference number, good oxidative stability, and, more importantly, an ultrafast self-healing behavior. The steady and dynamic rheological experiments conducted for the self-healing hydrogel polymer electrolyte have shown a healing efficiency of 93% within just 5 min. In the Zn||Zn symmetric cells, the HGPE suppresses the dendrite growth, enabling stable cycling for over 1000 h by maintaining high performance. In the coin cell, when the cell was tested with a Zn-doped MnO cathode, high discharge capacity could be achieved. The performance was further validated by integrating it into a rechargeable homemade pouch cell with a Zn-doped MnO cathode. Hence, the present work offers several promising advancements in the development of self-healing hydrogel polymer electrolytes for the flexible rechargeable zinc metal batteries.

A. In this work, we introduced a multifunctional hydrogel electrolyte that simultaneously tackles dendrite formation and cathode-anode crosstalk through the synergistic action of a chelating additive (EDTA) and a robust polyvinyl alcohol (PVA)-polyacrylic acid (PAA) polymer network. The article investigates a unified electrolyte design approach to concurrently inhibit the cathode-anode cross-talk and zinc dendrite formation in aqueous rechargeable zinc metal batteries (ARZMBs).