Vehicle-type ion transport and shuttle suppression enabled by a Zn²⁺-centered dual-ligand coordination hydrogel electrolyte toward highly reversible Zn-I₂ batteries.

Authors

Jiaxin Lv, Yi Shao, Ting Yao, Chen Xu, Xiubin Ren, Ying Yang, Yangyang Wang, Xiaojie Liu

Published in

Chemical science. Aug 07, 2026. Epub Aug 07, 2026.

Abstract

The practical deployment of aqueous Zn-I₂ batteries (AZIBs) is severely constrained by two tightly coupled issues: uncontrollable zinc dendrite growth and the shuttling of soluble polyiodides. To address this dual challenge, we engineer a multifunctional polymer hydrogel (PHE) electrolyte by integrating pyrrolidone carboxylate zinc (PCA) into a sulfonate-rich poly-(2-acrylamido-2-methylpropane sulfonic acid) (AMPS) network. This design forms a stable dual-ligand coordination complex, where carboxylate (-COO^-) and sulfonate (-SO₃ ^-) groups synergistically chelate Zn²⁺ ions, establishing a robust three-dimensional ion-conducting matrix. This architecture not only guides uniform Zn deposition by regulating Zn²⁺ solvation but also reconstructs the hydrogen-bonding network in the bulk, slowing proton mobility via a high-barrier vehicle-type mechanism. Meanwhile, Zn²⁺-centered electropositive domains strongly interact with polyiodide species (e.g., I₃ ^-), effectively immobilizing them and mitigating shuttle-induced corrosion. Together, this coordination-driven synergy enables concurrent regulation of Zn²⁺ transport, proton activity, and polyiodide capture within a single electrolyte system. As a result, the PHE endows Zn‖Zn symmetric cells with exceptional dendrite-free cycling stability over 2300 hours, enables a remarkably high coulombic efficiency of over 99.8% in Zn‖Cu asymmetric cells, and empowers Zn-I₂ full cells with outstanding longevity, exhibiting an ultralow capacity decay rate of 0.0018% per cycle over 10 000 cycles.

PMID:
42568974
Bibliographic data and abstract were imported from PubMed on 08 Aug 2026.

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