Densely Packed Li‐Metal Growth on Anodeless Electrodes by Li⁺‐Flux Control in Space‐Confined Narrow Gap of Stratified Carbon Pack for High‐Performance Li‐Metal Batteries

Abstract Lithium (Li) is the “holy grail” for satisfying the increasing energy demand. This is because of its high theoretical capacity and low potential. Although Li is considered as a potential anode material, dendritic Li growth and the limited electrochemical properties continue to hinder its practical application. Structure‐based self lithium ion (Li⁺) concentrating electrodes with high capacity and uniform Li⁺‐flux are recommended to overcome these shortcomings of Li. However, recent studies have been limited to structural perspectives. In addition, the electrokinetic principle of electrode materials remains a challenge. Herein, the space‐confinement‐based strategy is suggested for condensed Li⁺‐flux control in nanoscaled slit spaces that induce the dense Li growth on an anodeless electrode by using the stratified carbon pack (SCP). The micro/mesoporous slits of the SCP concentrate the electric field, which is strengthened by the space‐confined electric field focusing, resulting in the accumulation of Li⁺‐flux in the host. The accumulated Li⁺ in host sites enables a uniform Li deposition with high capacity at high current density stably. Furthermore, SCPs have great compatibility with LiNi_0.8Co_0.1Mn_0.1O₂ (NCM811) cathode, representing the outstanding full cell performance with Li deposited electrode which show the high specific of 115 mAh g⁻¹ at 4 C during 350 cycles.