Pit-Free Stripping in Discharge-Initiated Lithium Metal Batteries

Lithium metal anodes (LMAs) are indispensable for next-generation batteries, offering the highest theoretical capacity and the lowest electrochemical potential. Yet, discharge-initiated lithium metal batteries (LMBs), which begin cycling by stripping Li from a pristine LMA, face greater interfacial challenges than charge-initiated systems, including sporadic Li stripping, pit-induced heterogeneity, and early protection failure. Elevated Li utilization and lean electrolyte, both essential for achieving >450 Wh kg–1, exacerbate these interfacial challenges by promoting heterogeneous SEI formation and pit-driven Li pulverization. This Perspective revisits interfacial design principles by dissecting the distinct SEI formation mechanism under stripping conditions, clarifying the chemical and structural roles of the native LMA surface in pit nucleation, and evaluating bulk crystallographic texturing and scaffolding strategies for pit suppression. We propose a paradigm shift toward adaptive protection layers that conform to evolving interfaces, self-repair local defects, and redistribute the Li+ flux. These approaches offer a pathway to intelligently interactive, pit-free, dendrite-free LMAs for durable, energy-dense discharge-initiated LMBs.