摘要
Fragmented interfacial electron transfer amplifies localized electric fields and induces anisotropic Zn2+ diffusion, which ultimately culminates in heterogeneous nucleation and rampant dendrite growth. However, prevailing modification strategies are confined to passive suppression of deposition consequences, while disregarding the dynamic role of electron transport at the interface. Herein, we construct a ZnFe2O4 (ZFO) interlayer to actively modulate interfacial reaction behavior. The Zn@ZFO interlayer establishes a contiguous, low-impedance electron percolation network, facilitating lateral electron redistribution. This electron-percolation driven electric field regulation further induces a quasi-Ohmic softened interfacial response, effectively attenuating localized reaction amplification and synergistically coupling electron and Zn2+ fluxes. Furthermore, the hybrid nucleation growth regime arising from reduced Gibbs free energy contributes to the conformal distribution of Zn nuclei, mediating dense zinc deposition. Consequently, the Zn@ZFO modification creates a percolation-like electron-transport framework that minimizes interfacial resistance and accelerates carrier dynamics, enabling the Zn@ZFO symmetric cell to achieve ultra-long cycling stability (>4000 h) with a minimal hysteresis of 46.4 mV. Coupled with a V2O5 cathode, this modification promotes a kinetic transition from diffusion-controlled behavior to predominantly pseudocapacitive Zn2+ storage, thereby enabling high-rate performance at 5–10 A g−1. These results establish a physically grounded interfacial design strategy for stabilizing Zn metal anodes.
A ZnFe2O4 interlayer on Zn reprograms interfacial charge transport from localized hopping to a percolation-governed electron network. The resulting continuous electronic pathway homogenizes the interfacial electric field and intrinsically couples electron–Zn2+ flux, thereby regulating Zn nucleation behavior and suppressing dendritic growth for stable Zn metal anodes. [Display omitted]
•A ZnFe2O4 semiconductor interlayer regulates interfacial electron distribution for stable Zn anodes.•Hopping-mediated transport and electron percolation establish Ohmic-contact-assisted charge-transfer pathways.•Percolative electron redistribution homogenizes interfacial electric fields and suppresses localized Zn deposition.•The Zn@ZFO anode delivers ultrastable cycling over 4000 h with minimal voltage hysteresis.