Flexible and Dynamic Interfacial Desolvation in High-Entropy Electrolyte for Dendrite-Free Aqueous Zinc-Ion Batteries.
basic_science · Level V
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- Record sourced from PubMed, PMID 40970811.
- Also identified by DOI 10.1002/adma.202512633.
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Abstract
Aqueous zinc-ion batteries are promising candidates beyond lithium-ion technologies, but the intrinsic hydrogen-down orientation of interfacial water under negative bias, together with ion depletion at the electrode surface, promotes inhomogeneous Zn plating and substantial hydrogen evolution. Here, a high-entropy flexible electrolyte (HEFE) is demonstrated that leverages the fast water-exchange kinetics of Li⁺, K⁺, and Cs⁺. By deliberately inducing cation-hydration disequilibrium, the HEFE forms flexible Zn(H<sub>2</sub>O)<sub>m</sub> <sup>2+</sup> (m ≤ 6) solvation structures embedded in a disordered water network, enhancing ionic conductivity and alleviating ion-transport limitations. Under cathodic bias, a progressive desolvation from Zn(H<sub>2</sub>O)<sub>6</sub> <sup>2+</sup> to Zn(H<sub>2</sub>O)<sub>x</sub> <sup>2+</sup> (x ≤ 5) proceeds while retaining aqueous disorder, thereby suppressing hydrogen evolution and enabling 3500 h of deep cycling at 1 mA cm<sup>-2</sup>/3 mAh cm<sup>-2</sup>. For iodine cathodes, the HEFE induces a pathway shift from the conventional I<sup>-</sup>→I<sub>2</sub> route to a solid-solid (CsI→I<sub>2</sub>) conversion, fundamentally inhibiting iodide shuttling and extending full-cell life to 3600 cycles at 1 A g<sup>-1</sup>. Beyond Zn, the solvation-heterogeneity strategy opens avenues for reversible multivalent electrochemistry and advancing next-generation energy-storage systems.