Molecular Dipoles as a Surface Flattening and Interface Stabilizing Agent for Lithium‐Metal Batteries

Reaching the border of the capable energy limit in existing battery technology has turned research attention away from the rebirth of unstable Li‐metal anode chemistry in order to achieve exceptional performance. Strict regulation of the dendritic Li surface reaction, which results in a short circuit and safety issues, should be achieved to realize Li‐metal batteries. Herein, this study reports a surface‐flattening and interface product stabilizing agent employing methyl pyrrolidone (MP) molecular dipoles in the electrolyte for cyclable Li‐metal batteries. The excellent stability of the Li‐metal electrode over 600 cycles at a high current density of 5 mA cm(−2) has been demonstrated using an optimal concentration of the MP additive. This study has identified the flattening surface reconstruction and crystal rearrangement behavior along the stable (110) plane assisted by the MP molecular dipoles. The stabilization of the Li‐metal anodes using molecular dipole agents has helped develop next‐generation energy storage devices using Li‐metal anodes, such as Li–air, Li–S, and semi‐solid‐state batteries.