Abstract

The irreversible issues of Zn anode stemming from dendrite growth and water-induced erosion have severely hindered the commercialization of rechargeable aqueous Zn batteries. Herein, a hydrophobic and fast-Zn2+-conductive zinc hexacyanoferrate (HB-ZnHCF) interphase layer is in-situ integrated on Zn by a rapid room-temperature wet-chemistry method to address these dilemmas. Different from currently proposed hydrophilic inorganic cases, the hydrophobic and compact HB-ZnHCF interphase effectively prevents the access of water molecules to Zn surface, thus avoiding H2 evolution and Zn corrosion. Moreover, the HB-ZnHCF with large internal ion channels, strong zincophilicity, and high Zn2+ transference number (0.86) permits fast Zn2+ transport and enables smooth Zn deposition. Remarkably, the resultant HB-ZnHCF@Zn electrode delivers unprecedented reversibility with 99.88% Coulombic efficiency over 3000 cycles, realizes long-term cycling over 5800 h (> 8 months, 1 mA cm-2) and 1000 h (10 mA cm-2), and assures the stable operation of full Zn battery with both coin- and pouch-type configurations.

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