Uniform Zn Stripping/Plating Enable by PANI:PSS/Cellulose Framework for Dendrite-Free Rechargeable Aqueous Zinc-Ion Batteries

In this study, an artificial interfacial layer (PANI-C) for Zn anode consisting of hydrophilic cellulose nanocrystals and polyaniline was designed to address the dendrite growth problem at the electrode/electrolyte interface in aqueous Zn-ion batteries. Benefiting from the synergistic effect of high electronegativity and abundant surface functional groups, PANI-C accelerates the ordered migration of Zn2+, homogenizes the cosolvent of Zn2+ and effectively improves the reversibility of the zinc plating process, with strong zincophilicity and inhibition of dendrites. In addition, the PANI-C layer has abundant carbonyl adsorption sites uniformly distributed at the molecular level, and exhibits good ionic modulation ability during the Zn2+ plating/stripping process. The Zn||Cu asymmetric cell exhibited excellent reversibility with an average Coulombic efficiency of 99.3% after 1000 cycles at 1 mA cm–2. The assembled PANI-C@Zn//V2O5 full cell maintains 94.6% of its original capacity at 1 A g–1 after 2500 h, with an ultralong cycling time of 1500 h instantly even at a high current density of 5 A g–1. This strategy provides insight into the design of dendrite-free zinc anodes and highlights their applicability for practical zinc-based energy storage in the future.