The
essence of Zn dendrite formation is ultimately derived from
Zn nucleation and growth during the repeated Zn plating/stripping
process. Here, the nucleation process of Zn has been analyzed using
ex situ scanning electron microscopy to explore the formation of the
initial Zn dendrite, demonstrating that the formation of tiny protrusions
(the initial state of Zn dendrites) is caused by the inhomogeneity
of Zn nucleation. Based on this, the uniform Zn nucleation is promoted
by the Ni5Zn21 alloy coating (ZnNi) on the surface
of Zn foil by electrodeposition, and the mechanism of ZnNi-promoted
even nucleation is further analyzed with the assistance of density
functional theory (DFT). The DFT results indicate that the ZnNi displays
a stronger binding ability to Zn compared to the bare Zn, suggesting
that Zn nuclei will preferentially form around ZnNi instead of continuing
to grow on the surface of the initial Zn nuclei. Therefore, the designed
Zn metal anode (Zn@ZnNi) can be ultra-stable for over 2200 h at a
current density of 2 mA cm–2 in the symmetric cell.
Even at a much higher current density of 20 mA cm–2, the extra-long life of over 2200 cycles (over 530 h) can be achieved.
Moreover, the full cell with the Zn@ZnNi anode exhibits extra-long
cycling performance for 500 cycles with a capacity of 207.7 mA h g–1 and 1100 cycles (148.5 mA h g–1) at a current density of 0.5 and 1 A g–1, respectively.