LiZn/Li${}_2$O induced chemical confinement enabling dendrite-free Li-metal anode

Li metal has been considered as a potential anode candidate for next-generation high-energy Li-metal batteries, even though the uncontrollable growth of Li dendrites shortens their cycling lifespan. Herein, a reliable and dendrite-free Li-metal anode is fabricated via inducing chemical confinement based on an atomic layer deposited lithiophilic ZnO in situ generating LiZn/Li${}_2$O arrays. In a configuration, the arrays consisting of uniformly distributed LiZn and Li${}_2$O phases, the lithiophilic Li${}_2$O phases with favorable Li diffusion barrier guarantee the preferential Li nucleation and prevent the Li diffusion to some sites with uneven charge accumulation. Furthermore, these functional LiZn/Li2O configurations with satisfied localized free electron distribution can effectively decompose the Li clusters to prevent Li aggregation. Meanwhile, the electron-conductive LiZn phases ensure efficient electron transfer throughout the configuration. Therefore, the LiZn/Li${}_2$O-derived chemical confinement enables uniform Li deposition. Consequently, the as-prepared Li-metal anode presents an overpotential <45 mV at 15 mA cm${}^{-2}$ in the symmetrical cells. Moreover, the preferable cycling stability and rate capability are delivered by the as-assembled cells with a LiNi${}_{0.6}$Co${}_{0.2}$Mn${}_{0.2}$O${}_2$ (NCM622) cathode. It is believed that the strategy proposed here can be also beneficial to other effective chemical confinement systems for fabricating high-performance Li metal anode. (© 2023 Wiley‐VCH GmbH)