Hydrated Network Interphase with Dynamic Negatively Charged Microregion Enables Ultra-Stable Aqueous Zinc-Ion Batteries
Corresponding Author: Houzhao Wan
Nano-Micro Letters,
Vol. 18 (2026), Article Number: 418
Abstract
Aqueous zinc-ion batteries are promising candidates for large-scale energy storage, yet their development is severely hindered by the interfacial instability of zinc anodes. Distinct from strategies employing pre-formed polymers, this work proposes an innovative monomer-induced in situ interface engineering strategy. By leveraging the preferential adsorption of acrylamide monomers on the Zn surface, a locally high-concentration region is created, which subsequently enables the in situ construction of a stable hydrated network interphase (HNI) triggered synergistically by Zn2+ and SO42− during electrochemical cycling. The HNI precisely regulates Zn deposition via a triple synergistic mechanism: Lewis acid–base coordination (C = O···Zn2+) provides fixed nucleation sites; dynamically anchored SO42− within the interphase forms negatively charged microregions that homogenize Zn2+ flux via Coulombic repulsion; and a dense hydrogen-bonding network effectively confines free water and suppresses side reactions. Benefiting from this multifunctional interphase, the Zn//Zn symmetric cell achieves an ultra-long cycling life of 8650 h (over 360 days) at 1 mA cm−2 with excellent reproducibility, the Zn//Ti cell delivers a high average Coulombic efficiency of 99.71% at 5 mA cm−2. The Zn//I2 full cell retains 89.15% of its capacity after 12,000 cycles. This work provides a novel paradigm for interfacial construction toward high-performance zinc metal anodes.
Highlights:
1 A hydrated network interphase with dynamic negatively charged microregions is constructed in situ via electrochemically triggered Zn2+/SO42– synergy, enabling triple synergistic regulation of Zn deposition.
2 The HNI-modified Zn anode achieves ultra-long cycling (8650 h at 1 mA cm–2 and 1600 h at 10 mA cm–2) and high Coulombic efficiency (99.71%).
3 The Zn//I2 cell delivers a high specific capacity of 356.27 mAh g–1 at 1 A g–1 and retains 89.15% capacity after 12,000 cycles.
Keywords
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