Unraveling Paradoxical Effects of Large Current Density on Zn Deposition

Abstract Aqueous zinc‐based batteries (ZBs) have been widely investigated owing to their intrinsic safety, low cost, and simple assembly. However, the actual behavior of Zn deposition under large current density is still a severe issue associated with obscure mechanism interpretation of ZBs under high loading. Here, differing from the conventional understanding that short circuit is induced by dendrite penetrating under large current density (10–100 mA cm⁻²), the separator permeation effect is unraveled to illustrate the paradox between smooth deposition and short lifespan. Generally, a dense plating morphology is achieved under large current density because of intensive nuclei and boosted plane growth. Nevertheless, in the scenes applying separators, the multiplied local current density derived from narrow separator channels leads to rapid Zn²⁺ exhaustion, converting the Zn deposition mode from nucleation control to concentration control, which eventually results in separator permeation and short circuit. This effect is validated in other aqueous metal anodes (Cu, Sn, Fe) and receives similar results. Based on the understanding, a micro‐pore (150 µm) sponge foam is proposed as separators for large‐current anodes to provide broader Zn²⁺ path and mitigate the separator permeation effect. This work provides unique perspectives on coordinating fast‐charging ability and anode stability of ZBs.