Toward High‐Performance Zn Anodes: A Synergistic Dual‐Ion Strategy via Interfacial Orientation Optimization

ABSTRACT Aqueous zinc metal batteries (AZMBs) demonstrate compelling advantages of low cost, high safety, and environmental benignity, rendering them promising candidates for next‐generation energy storage systems. However, their commercialization is impeded by irreversible Zn anode issues, including dendrite growth, interfacial corrosion, and parasitic side reactions. This work introduces sodium tartrate (NTA) as a dual‐ion additive that mitigates these challenges via cationic (Na + ) electrostatic shielding and anionic (TA 2− ) acceleration of [Zn(H 2 O) 6 ] 2+ desolvation, guiding uniform (002)‐oriented Zn deposition. Such a deposition orientation facilitates the uniform nucleation of Zn 2+ on the Zn anode. Leveraging the synergistic adsorption protection of Na + and TA 2− , this mechanism ultimately enables a highly reversible Zn anode. Results confirm the Zn symmetric cell with modified electrolyte achieves stable reversible Zn plating/stripping for over 3000 h at 6.0 mA cm −2 /1.0 mAh cm −2 . Moreover, the Zn||Cu asymmetric cell exhibits exceptional cycling stability, delivering an average coulombic efficiency (CE) of 99.81% over 2900 cycles at 1.0 mA cm −2 /0.5 mAh cm −2 and 99.82% over 3000 cycles at 5.0 mA cm −2 /1.0 mAh cm −2 . The NTA additive also demonstrates outstanding electrochemical compatibility in both Zn||α‐MnO 2 and Zn||I 2 full cells. Notably, the Zn||I 2 full cell maintains a high capacity retention of 93.29% after 10 000 cycles at 5.0 A g −1 , highlighting its practical potential.