Yanguo Liu

Severe zinc dendrite growth and parasitic side reactions significantly limit the cycling stability of aqueous zinc-ion batteries (AZIBs), hindering their practical application. Herein, we propose a rational strategy to regulate Zn deposition by engineering protective layers with distinct Zn coordination environments. By precisely tailoring the coordination states of Zn atoms, heterogeneous interfacial microenvironments are constructed, which synergistically suppress dendrite formation and the hydrogen evolution reaction (HER). Specifically, low-coordinated Zn sites enhance zincophilicity, enabling uniform Zn nucleation and deposition, while high-coordinated Zn sites weaken H adsorption and effectively inhibit HER. As a result, the Zn-0.55N2+0.45N3@Zn||Zn-0.55N2+0.45N3@Zn symmetric cell achieves an ultralong cycling lifespan of 6322 h at 1 mA cm-2. Meanwhile, the Zn-0.55N2+0.45N3@Zn||MnO₂ full cell exhibits markedly improved cycling stability and rate capability. This work establishes a clear correlation between atomic coordination environments and interfacial electrochemical behavior, offering a new design paradigm for highly reversible Zn anodes in next-generation AZIBs.

Spontaneous redox reaction between the defective TiO₂ powder and the oxidative graphene oxide (GO) substate can be used to form the interface covalent bonds in the composites, which are responsible for the enhancement of lithium storage performance.