Multi-component gradients in 3D host frameworks enabled stack-type zinc plating/stripping for highly durable aqueous Zn-ion batteries.

Sun, Jingjie; Shen, Tianyu; Zhang, Mingyue; Xing, Yizhi; Wei, Jie; Yu, Qianchuan; Tie, Zuoxiu; Jin, Zhong · Sci Adv · 2026

basic_science · Level V

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Abstract

Developing dendrite-free zinc metal anodes with high durability poses a great challenge for aqueous zinc-ion batteries. Herein, we propose an in situ constructed 3D restrained host frameworks with multi-component gradients that induces a controllable and rapid stack-type zinc plating/stripping behavior, enabling a unique "first-in/last-out" mode. Typically, hydrophobic amino-functionalized polysilane passivation layer and zincophilic Ag nanoparticles are successively self-assembled on carbon paper scaffold to form opposite concentration gradients, namely <i>g'</i>-Ag/<i>g</i>-PSiO<sub>x</sub>-NH<sub>2</sub>/CP. The <i>g</i>-PSiO<sub>x</sub>-NH<sub>2</sub> inhibits side-reactions and promotes Zn<sup>2+</sup> desolvation, meanwhile the <i>g'</i>-Ag guides preferential Zn<sup>2+</sup> deposition. Consequently, the zinc-deposited <i>g'</i>-Ag/<i>g</i>-PSiO<sub>x</sub>-NH<sub>2</sub>/CP electrodes exhibit high Coulombic efficiency and long cyclability, surpassing 5000 hours at 10 mA cm<sup>-2</sup>/10 mAh cm<sup>-2</sup> in symmetric cells. The as-assembled Zn||MnO<sub>2</sub> full batteries deliver a specific capacity of 200.1 mAh g<sup>-1</sup> with 82.2% retention after 800 cycles. Large-size pouch-type battery with zinc-deposited <i>g'</i>-Ag/<i>g</i>-PSiO<sub>x</sub>-NH<sub>2</sub>/CP anode and high-loading MnO<sub>2</sub> cathode (∼15 mg cm<sup>-2</sup>) also exhibit good rate capability and cyclability. This scalable strategy offers a feasible solution to develop high-durability rechargeable metal-based batteries.