Hierarchical Confinement Effect with Zincophilic and Spatial Traps Stabilized Zn-Based Aqueous Battery

Abstract

Zn-based aqueous batteries (ZABs) have been regarded as promising candidates for safe and large-scale energy storage in the "post-Li" era. However, kinetics and stability problems of Zn capture cannot be concomitantly regulated, especially at high rates and loadings. Herein, a hierarchical confinement strategy is proposed to design zincophilic and spatial traps through a host of porous Co-embedded carbon cages (denoted as CoCC). The zincophilic Co sites act as preferred nucleation sites with low nucleation barriers (within 0.5 mA h cm^-2), and the carbon cage can further spatially confine Zn deposition (within 5.0 mA h cm^-2). Theoretical simulations and <i>in situ</i>/<i>ex situ</i> structural observations reveal the hierarchical spatial confinement by the elaborated all-in-one network (within 12 mA h cm^-2). Consequently, the elaborate strategy enables a dendrite-free behavior with excellent kinetics (low overpotential of <i>ca</i>. 65 mV at a high rate of 20 mA cm^-2) and stable cycle life (over 800 cycles), pushing forward the next-generation high-performance ZABs.