Synergy of Dendrites-Impeded Atomic Clusters Dissociation and Side Reactions Suppressed Inert Interface Protection for Ultrastable Zn Anode.

Abstract

The sluggish ions-transfer and inhomogeneous ions-nucleation induce the formation of randomly oriented dendrites on Zn anode, while the chemical instability at anode-electrolyte interface triggers detrimental side reactions. Herein, this report in situ designs a multifunctional hybrid interphase of Bi/Bi₂O₃, for the first time resulting in a novel synergistic regulation mechanism involving: (i) chemically inert interface protection mechanism suppresses side reactions; and more fantastically, (ii) innovative thermodynamically favorable Zn atomic clusters dissociation mechanism impedes dendrites formation. Assisted by collaborative modulation behavior, the Zn@Bi/Bi₂O₃ symmetry cell delivers an ultrahigh cumulative plating capacity of 1.88 Ah cm^-2 at 5 mA cm^-2 and ultralong lifetimes of 300 h even at high current density and depth of discharge (10 mA cm^-2, DOD_Zn: 60%). Furthermore, under a low electrolyte-to-capacity ratio (E/C: 45 µL mAh^-1) and negative-to-positive capacity ratio (N/P: 6.3), Zn@Bi/Bi₂O₃||MnO₂ full-cell exhibits a superior capacity retention of 86.7% after 500 cycles at 1 A g^-1, which outperforms most existing interphases. The scaled-up Zn@Bi/Bi₂O₃||MnO₂ battery module (6 V, 1 Ah), combined with the photovoltaic panel, presents excellent renewable-energy storage ability and long output lifetime (12 h). This work provides a fantastic synergistic mechanism to achieve the ultrastable Zn anode and can be greatly promised to apply it into other metal-based batteries.