Synergistic Modulation of Zn Anode via Ferroelectric and Zincophilic Cr‐Doped ZnO Interface

Abstract The unstable zinc anode hinders the practical application of aqueous zinc‐ion batteries, primarily due to two interconnected issues: dendrite formation induced by the kinetic‐controlled plating model and side reactions resulting from the thermodynamic‐driven hydrogen evolution. Herein, a multifunctional interface, composed of Cr‐doped ZnO (CZO) nanoparticles integrated with polyvinylidene difluoride (PVDF), stabilizes the zinc anode (CZO@Zn). Introducing ferroelectricity into CZO through Cr doping ensures a uniform electric field distribution, promoting thermodynamic‐favored epitaxial growth. The zincophilicity of CZO increases nucleation sites, while its hydrophobicity effectively suppresses side reactions. By optimizing both thermodynamics and kinetics, a “concrete‐slab”‐like deposition is achieved even under high areal capacity and rate conditions. The CZO layer enables high zinc reversibility (99.97%), long‐term stability (2400 h), and a high zinc utilization rate (80%). CZO‐modified separator exhibits an exceptionally long‐term lifespan of 2800 h. This approach can be extended to the design of a V‐doped ZnO interface. The ferroelectric–zincophilic interlayer offers distinct advantages over traditional ferroelectric materials and pure ZnO, making it a promising alternative for stabilizing the zinc anode.