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

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 g’ -Ag/ g -PSiO _x -NH ₂ /CP. The g -PSiO _x -NH ₂ inhibits side-reactions and promotes Zn ²⁺ desolvation, meanwhile the g’ -Ag guides preferential Zn ²⁺ deposition. Consequently, the zinc-deposited g’ -Ag/ g -PSiO _x -NH ₂ /CP electrodes exhibit high Coulombic efficiency and long cyclability, surpassing 5000 hours at 10 mA cm ⁻² /10 mAh cm ⁻² in symmetric cells. The as-assembled Zn||MnO ₂ full batteries deliver a specific capacity of 200.1 mAh g ⁻¹ with 82.2% retention after 800 cycles. Large-size pouch-type battery with zinc-deposited g’ -Ag/ g -PSiO _x -NH ₂ /CP anode and high-loading MnO ₂ cathode (∼15 mg cm ⁻² ) also exhibit good rate capability and cyclability. This scalable strategy offers a feasible solution to develop high-durability rechargeable metal-based batteries.