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Aqueous Metal-Anode Deposition and Dendrite Suppression

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Synergetic Effect of Multicomponent Phosphate and Rich Grain-Boundary in Solid/Electrolyte Interphase Boosts Rapid Ion Transport Toward Fast Aqueous Zinc Metal Batteries

The development of fast-charging aqueous zinc (Zn) metal batteries is crucial for large-scale energy storage applications. However, in pursuit of fast-charging capability under a high current density (>10 mA cm−2), the intensified Zn2+ flux imbalance at the electrolyte/anode interphase will cause more uncontrolled dendrite growth. Herein, with experimental and simulation results, a theoretical formulation is proposed to reveal a current density-dependent failure mechanism that elucidates how space-charge-induced Zn2+ accumulation triggers cascading dendrite formation. To mitigate this kinetic mismatch, a fast-ion-conducting solid/electrolyte interphase (SEI) model system with multicomponent phosphate and rich grain-boundary is established, by which the Zn2+ transference number increases from 0.25 to 0.82 and the migration energy barrier at the interphase decreases from 3.80 to 1.35 eV. Consequently, this designed interfacial remodeling enables Zn||Zn cells to exhibit ultrahigh-rate capability and extended durability (achieving 13 000 cycles at 40 mA cm−2 and 4000 h at 0.5 mA cm−2). More significantly, full cells retain 86% capacity after 2000 cycles at 2 A g−1, while industrial-scale 4 × 6 cm2 pouch cells maintain 90.3% capacity over 100 cycles. Collectively, these findings establish a universal interfacial design principle for high-power aqueous metal batteries by correlating grain-boundary ion dynamics with effective dendrite suppression.

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