Grid Shielding of Interphase Hybrids Via Spatial Charge Separation for Regulating Interfacial Zn Redox Kinetics

The ongoing dilemma of Zn metal anodes stems from rampant dendrite growth and persistent side reactions, which hinder their practical application in next-generation aqueous energy storage systems. Herein, spatial charge separation is achieved with the cross-linked Zn2+-affinity interfacial host to stabilize Zn anode chemistry. Enriched zincophilicity arises from the ideal distribution of binary Cu-Sn metallic nanodomains with textured facets, which readily serve as preferential sites with lowered Zn nucleation barrier. The carbonaceous nanoarchitecture promotes a uniform local current density during Zn2+ plating/stripping, affording both volume accommodation and spatial confinement of Zn deposits. Notably, a well-defined electrostatic shielding effect with an atomically grid-unit pattern is established through interfacial charge redistribution, which is enabled at the heterointerface between electrically conductive carbon sheet and Cu-Sn alloy nanoparticles as the electron acceptor. This configuration regulates Zn2+ diffusion pathways and promotes redox kinetics, resulting in a low voltage hysteresis of 17 mV over 4800 h (exceeding 6 months) with the interphase hybrids. The resulting Zn-ion full cells demonstrate stable cycling performance over 1500 cycles at 2 A/g.