Inducing (101)-preferred orientation in Zn metal anodes via texture engineering for dendrite-free aqueous Zn-ion batteries

Abstract

Conventional aqueous zinc-ion batteries (AZIBs) face critical challenges, including dendritic growth, interfacial corrosion, and parasitic side reactions, which severely limit their long-term reversibility. In this work, a grain orientation transition strategy is proposed to intrinsically stabilize Zn metal anodes through controlled thermal annealing and mechanical roll-pressing. The approach begins with fabricating Zn foils dominated by the (101) crystallographic plane, which subsequently evolves toward a thermodynamically stable (002) texture during cycling. Comprehensive EBSD, BC imaging, and pole figure analyses reveal that annealing-induced grain coarsening and deformation-driven grain refinement collectively regulate the initial microstructure and its dynamic orientation evolution. Unlike conventional (002)-oriented or fine-grained Zn foils that undergo severe morphological degradation, the engineered (101)-oriented Zn exhibits a uniform and compact Zn deposition morphology, benefiting from its favorable nucleation characteristics and cycling-induced transition to the stable basal plane. Symmetric cell tests demonstrate significantly enhanced reversibility, with stable cycling exceeding 500 h at 2 mA cm−2 and 2 mAh cm‐2 and more than 1200 h at 1 mA cm‐2. Full cells paired with an I2@ACC cathode maintain stable cycling over 900 cycles at 1 A g‐1 with reduced voltage hysteresis. These results validate grain orientation transition as an effective and scalable strategy for enabling dendrite-free Zn deposition and highlight its potential for the practical development of next-generation AZIBs.