A Facile Superlithiophilic 3d Host with Transition Metal Oxides Heterostructure for Ultrastable Zero-Volume-Expansion Lithium Metal Anodes

Abstract

Lithium metal batteries (LMBs) have garnered immense attention as the frontrunners for next-generation energy devices due to their unprecedented capacity and the lowest electrochemical potential in nature. Nonetheless, their practical implementation has been hindered by critical challenges, including dendrite formation and the instability of the solid electrolyte interface (SEI). In this study, we present a pioneering in-situ growth of a ZnO-CuO heterostructure in a crack shield construction on a three-dimensional (3D) copper foam host. Computational COMSOL simulations reveal marked improvements in electron transfer processes post-decoration. In galvanostatic measurements, the Li@ZnO-CuO-CF electrode demonstrates exceptional stability, exhibiting only a 0.2 V hysteresis and no volume expansion in a symmetric cell under a 50 mA cm-2 current density. Moreover, the electrode retains a remarkable 95.4% of its initial capacity after 600 cycles at 0.5 C and an impressive 85.5% capacity after 220 cycles at 1 C when paired with a high-loading LiFePO4 (LFP) cathode. These findings underscore the substantial potential of our well-designed electrode as a significant advancement in LMB development.

Keywords: Lithium metal anodes, Crack shield construction, ZnO-CuO heterostructure, Uniform deposition