Regulating Zn2+ Desolvation and (002)-Oriented Deposition for Stable Zinc Metal Anodes

Dendrite growth and interfacial side reactions of zinc metal anodes severely constrain the practical application of aqueous zinc-ion batteries (AZIBs). Here, a simple and well-established strategy is proposed by constructing a polyimide/UiO-66-NH2 composite interlayer (Zn@PI-UiO-66-NH2) with a three-dimensional porous structure on the surface of zinc foil via electrospinning followed by thermal imidization. This interlayer integrates the mechanical stability of polyimide with the chemical functionality of UiO-66-NH2, enabling precise regulation of zinc deposition behavior through multiple synergistic mechanisms. The three-dimensional conductive network of polyimide and well-defined porous channels of UiO-66-NH2 with functional amino group effectively homogenizes the electric-field distribution and guides the preferential growth of zinc along the (002) crystal plane, thereby suppressing both dendrite formation and parasitic side reactions. Consequently, the modified zinc anode achieves long-term stable plating/stripping under various current densities, and exhibits enhanced cycling stability at high current densities when assembled into symmetric cells. The full cell with Zn@PI-UiO-66-NH2 anode and NaV3O8·1.5H2O cathode delivers a high discharge capacity and superior capacity retention. This work not only provides an efficient organic–inorganic hybrid interface engineering strategy but also offers unique insights into the rational design of high-performance zinc metal anodes, shedding light on the scale-up of advanced aqueous zinc-ion battery technology.