Process‐Oriented Interphase Regulation in Lithium Metal Batteries with Non‐Aqueous Liquid Electrolytes

ABSTRACT Lithium metal batteries (LMBs) are promising candidates for high‐energy‐density energy storage systems. However, their practical applications are severely hindered by interfacial instability and uncontrolled lithium deposition, which lead to dendrite growth, low Coulombic efficiency, and rapid capacity decay. In this review, we systematically analyze interfacial processes in LMBs with non‐aqueous liquid electrolytes from a process‐oriented perspective. We employ a six‐step kinetic framework involving ion transport, desolvation, interphase transport, charge transfer, nucleation, and morphological evolution. We first discuss the fundamental structure and dynamic evolution of electrode‐electrolyte interphases, followed by an overview of advanced characterization techniques across multiple length and time scales. Furthermore, recent strategies for regulating interfacial stability are critically summarized, including electrolyte additives, artificial protective layers, and solvation regulation designs. Instead of categorizing these strategies solely by materials, we emphasize their roles in regulating key kinetic steps and clarify the underlying mechanisms within the six‐step process. Finally, we highlight current challenges and future directions toward practical LMBs, including full‐cell and pouch‐cell validation, high energy density, cost reduction, and manufacturing compatibility. This work aims to provide a unified framework for understanding, characterizing, and regulating interfacial stability in lithium metal batteries.