Geometry-Regulated Electrode-Wide Nucleation Patterns in Aqueous Zinc Anodes

Zinc metal is a promising anode for aqueous zinc batteries due to its high theoretical capacity and low cost. However, its practical implementation remains limited by dendrite formation and interfacial instability. Herein, we present a geometry-driven strategy that regulates Zn deposition through control of the hole opening ratio (HOR) in laser-ablated three-dimensional hole-patterned Zn foil. Based on preferential Zn deposition at periodically arranged hole edges, HOR was introduced as a geometric parameter that dictates the spatial density of nucleation sites. Systematic variation of the HOR reveals that it governs the dispersion and size of early-stage Zn deposits, defining the electrode-wide nucleation pattern and subsequent growth behavior. The optimized HOR balances sparse nucleation with localized growth and dense nucleation with coalescence-driven aggregation, enabling spatially uniform Zn deposition. As a result, the HOR-tailored electrode achieves dendrite-free deposition with long-term stability in symmetric cells (3400 h at 0.5 mA cm^-2) and maintains stable cycling in full cells paired with a Zn pre-intercalated NH₄V₄O₁₀ cathode (1000 cycles at 2 A g^-1). By establishing HOR-controlled nucleation density as a geometry-based design principle, this defect-engineered and materials-independent approach provides a general design framework for high-performance aqueous metal batteries.