Electrochemo‐Mechanical Reinforcement of Zinc Powder Anodes Enables Tab‐Robust Aqueous Zinc Pouch Cells

ABSTRACT

Scaling aqueous zinc metal batteries from coin cells to practical pouch cells is hindered not only by parasitic interfacial reactions, but also by chemo‐mechanical coupling between heterogeneous Zn deposition and structural brittleness, which accelerates localized degradation and triggers pouch failure. Herein, a chemo‐mechanically reinforced zinc powder anode (ZP‐R@AA) is developed by reconstructing commercial Zn powders into a rigid porous framework and integrating a conformal ion‐regulating interphase. Multiscale analyses, including density functional theory, molecular dynamics, COMSOL simulation, electrochemical kinetics, and time‐of‐flight secondary ion mass spectrometry, reveal that this structure‐interface synergy homogenizes Zn ²⁺ transport and local electric‐field distribution, lowers deposition barriers, suppresses corrosion, and mitigates stress concentration, thereby interrupting the positive feedback between interfacial instability and mechanical damage. Consequently, the reinforced anode enables durable Zn plating/stripping for over 4100 h, far exceeding Zn foil. More importantly, post‐mortem analysis identifies tab fracture as a dominant scale‐up failure mode, which is effectively mitigated by ZP‐R@AA. The anode further enables 4.23 Ah Zn||VO ₂ pouch cells with 65% capacity retention after 1000 cycles and reduced raw‐material cost, establishing a practical structure‐interface design principle for durable aqueous zinc pouch batteries.