Synergizing Zincophilicity and Hydrophobicity via PVP–ZnO/PDMS Coating for Highly Reversible Zn Metal Anodes for Aqueous Zinc‐Ion Batteries

Aqueous zinc‐ion batteries are promising candidates for grid‐scale energy storage applications because of their high safety, low cost, and abundant raw materials. Nevertheless, their practical implementation is hindered by uncontrollable dendrite growth and parasitic side reactions at the Zn metal anode. Thus, herein, we propose a surface modification strategy using a multifunctional coating layer composed of hydrophobic polydimethylsiloxane (PDMS), zincophilic zinc oxide (ZnO), and polyvinylpyrrolidone (PVP; as a stabilizer). The PDMS matrix serves as a durable hydrophobic barrier, restricting direct contact between the Zn surface and the aqueous electrolyte and efficiently suppressing the hydrogen evolution reaction (HER). Concurrently, ZnO acts as the preferred nucleation site, lowering the nucleation overpotential and promoting uniform Zn deposition, whereas PVP ensures stable ZnO dispersion within the polymer matrix. As a result, PVP–ZnO/PDMS‐coated Zn symmetric cells exhibit outstanding cycling stability for over 1000 h at a current density of 5 mA cm ⁻² . Additionally, α‐MnO ₂ ||Zn cells with the modified anode exhibit improved capacity retention and a high Coulombic efficiency (CE) after an initial electrochemical activation. This dual‐functional coating is a simple and effective solution for the design of high‐performance anodes for durable, high‐energy aqueous energy storage systems.