Anion Vacancy Engineering of ZIF‐8‐derived ZnSe for Dendrite‐Free Zn Anodes

ABSTRACT Zinc (Zn) metal anodes face notorious side reactions and uncontrollable Zn dendrite growth, which severely hinders the commercialization of aqueous Zn metal batteries (AZMBs). Herein, we design a core‐shell zeolitic imidazolate framework‐8 precursor‐derived 3D nitrogen‐doped porous carbon (NPC) shell with an interior scattered selenium (Se) vacancy‐modified ZnSe nanoparticle interfacial layer on the Zn electrode, denoted V Se ‐ZnSe‐400@NPC‐Zn, to achieve homogeneous Zn deposition and superior anticorrosion capability. The inner dispersed zincophilic V Se ‐ZnSe‐400 nanoparticles enhance the Zn ion reaction kinetics and energy barriers for the hydrogen evolution reaction, as well as the rearrangement of the local electric field, thereby facilitating uniform Zn deposition and inhibiting side reactions. Meanwhile, the well‐developed dodecahedra NPC can provide Zn ion regulation channels and alleviate volume expansion, which further suppresses the formation of Zn dendrites. Consequently, the V Se ‐ZnSe‐400@NPC‐Zn//V Se ‐ZnSe‐400@NPC‐Zn symmetric cell exhibits a superior cycling lifespan of over 2000 h at 1.0 mA cm −2 /1.0 mAh cm −2 . Moreover, benefiting from the stable V Se ‐ZnSe‐400@NPC‐Zn electrode, the assembled Zn//I 2 full cell maintains an outstanding stability of more than 6000 cycles at 2.0 C. This research provides a surface modification strategy based on structure and vacancy engineering for the practical application of next‐generation AZMBs.