Orbital‐Hybridizable Nanoseed Interphase Enables One‐Minute Rechargeable, Energy‐Dense Anode‐Free Aqueous Zinc Batteries

Aqueous zinc (Zn) batteries are emerging as promising candidates for energy storage systems (ESS) and wearable electronics, but their practical application is hindered by low energy density and electrochemical instability at the Zn anode–electrolyte interface. Here, we report an orbital-hybridizable nanoseed (OHNS) interphase composed of graphene oxide nanoribbons (GONRs) uniformly deposited on Cu current collectors via a scalable slot-die coating process, enabling one-minute-rechargeable, energy-dense anode-free aqueous Zn batteries. The carbon edges (C-edges) prevalent in the GONR facilitate orbital hybridization with Zn. This chemical interplay between the heteroatoms (C-edge and Zn) enhances Zn nucleation kinetics and retards surface diffusion of adsorbed Zn, thereby promoting corrosion-resistant, (002)-oriented growth of Zn. Consequently, reversible Zn plating/stripping with high Coulombic efficiency (∼99.5%) was achieved even at a high current density of 120 mA cm$^{−2}$. Moreover, anode-free full cells with the OHNS interphase delivered a maximum energy/power density of 140.6 Wh kg$^{−1}$/4138.1 W kg$^{−1}$. Notably, anode-free pouch cells exhibited stable capacity retention of 82.2% after 800 cycles at a fast charge/discharge current density of 106C (equivalent to a time of 34 s).