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Breaking Solid-Solid Conversion Barriers in Aqueous Zn-S Batteries via Dynamic Iodide Coordination and Solvation Regulation
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DOI：10.1002/adfm.202510149.png)
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Abstract
En 中文
Aqueous Zn-S batteries face challenges of sluggish S/ZnS conversion, parasitic reactions, and Zn dendrites. Herein, a dual-functional electrolyte integrating choline iodide (ChI) and ethylene glycol dimethyl ether (DME) is designed to synergistically enhance reaction kinetics and interfacial stability. The I−/I3− redox couple in ChI mediates sulfur conversion through coordination intermediates, lowering the ZnS oxidation barrier, while choline cations homogenize Zn2+ flux to suppress dendrites. Meanwhile, DME reconstructs Zn2+ solvation shells into stabilized [Zn(DME)0.04(H2O)5.32(OTF−)0.64]1.36+ complexes via ether oxygen coordination, reducing desolvation energy. Its hydrophobic nature further inhibits water-induced sulfate byproducts at the sulfur cathode. The optimized electrolyte enables a Zn-S battery to deliver a high capacity of 1507.7 mAh g−1 at 0.1 A g−1 and exceptional cycling stability (88.9% capacity retention after 800 cycles at 4 A g−1). A flexible quasi-solid-state Zn-S battery demonstrates robust mechanical durability (83.3% capacity retention after 400 cycles under folding/cutting) and powers electronic devices, highlighting its practicality. This work provides a synergistic electrolyte design strategy to unlock high-energy, long-cycling Zn-S batteries for scalable energy storage.
Keywords:
aqueous Zn-S batteries
cosolvent
electrolyte
redox mediator
synergy