Achieving Long-Cycle-Life Zinc-Ion Batteries through a Zincophilic Prussian Blue Analogue Interphase

Abstract

The practical application of rechargeable aqueous zinc-ion batteries (ZIBs) has been severely hindered by detrimental dendrite growth, uncontrollable hydrogen evolution, and unfavorable side reactions occurring at the Zn metal anode. Here, we applied a Prussian blue analogue (PBA) material K2Zn3(Fe(CN)6)2 as an artificial solid electrolyte interphase (SEI), by which the plentiful -C≡N- ligands at the surface and the large channels in the open framework structure can operate as a highly zincophilic moderator and ion sieve, inducing fast and uniform nucleation and deposition of Zn. Additionally, the dense interface effectively prevents water molecules from approaching the Zn surface, thereby inhibiting the hydrogen-evolution-resultant side reactions and corrosion. The highly reversible Zn plating/stripping is evidenced by an elevated Coulombic efficiency of 99.87% over 600 cycles in a Zn/Cu cell and a prolonged lifetime of 860 h at 5 mA cm−2, 2 mAh cm−2 in a Zn/Zn symmetric cell. Furthermore, the PBA-coated Zn anode ensures the excellent rate and cycling performance of an α-MnO2/Zn full cell. This work provides a simple and effective solution for the improvement of the Zn anode, advancing the commercialization of aqueous ZIBs.