<p>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 Zn<sup>2+</sup> and SO<sub>4</sub><sup>2−</sup> during electrochemical cycling. The HNI precisely regulates Zn deposition via a triple synergistic mechanism: Lewis acid–base coordination (C = O···Zn<sup>2+</sup>) provides fixed nucleation sites; dynamically anchored SO<sub>4</sub><sup>2−</sup> within the interphase forms negatively charged microregions that homogenize Zn<sup>2+</sup> 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&#xa0;days) at 1&#xa0;mA&#xa0;cm<sup>−2</sup> with excellent reproducibility, the Zn//Ti cell delivers a high average Coulombic efficiency of 99.71% at 5&#xa0;mA&#xa0;cm<sup>−2</sup>. The Zn//I<sub>2</sub> 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.</p><p></p>

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Hydrated Network Interphase with Dynamic Negatively Charged Microregion Enables Ultra-Stable Aqueous Zinc-Ion Batteries

  • Yin Yang,
  • Xiaofang Wang,
  • Xin Chen,
  • Jia Yao,
  • Daigan Wang,
  • Luyang Ge,
  • Fei Wang,
  • Lin Lv,
  • Li Tao,
  • Hao Wang,
  • Houzhao Wan

摘要

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.