Organic–Inorganic Nanoarchitectonics of Binder-Free Hybrid Protective Layer for Suppression of Dendrite Formation and Side Reactions with Stabilizing Zn Anodes

Aqueous Zn-ion batteries (AZIBs) are regarded as an attractive option for energy storage, given their superior safety, affordability, and environmental sustainability. Nevertheless, dendrite proliferation and persistent side reactions hamper the commercial deployment of Zn anodes, adversely affecting their Coulombic efficiency and overall cycling performance. Herein, we designed a stabilized Zn anode by depositing a binder-free hybrid protective layer constituted of a titanium phosphate (TiP) framework and chitosan (CS). The rigid TiP frameworks with ion channels can effectively induce uniform deposition of Zn2+ to suppress Zn dendrite growth. In addition, the −OH and -NH3 groups in CS provide Zn-affinitive sites for the rapid capture of Zn2+. This organic–inorganic structure is found to effectively prolong the lifetime of the Zn anode. The experiments reveal that the TiP-CS1:1@Zn symmetric cell shows superior cycling performance of 2600 h at 5 mA cm–2 current density and 1 mAh cm–2 charge capacity. Additionally, a high-capacity retention of 82.07% after 1000 cycles at 5 A g–1, coupled with a nearly 100% Coulombic efficiency, demonstrates the superior cycling stability of the TiP-CS1:1@Zn//MnO2 full cell. By presenting a facile yet effective approach for stabilizing Zn anodes, this work facilitates the advancement of high-performance AZIBs toward practical application.