Correlating the Potential-Holding Formation Protocol of Solid–Electrolyte Interphases with Improving Calendar Aging on Lithium Metal Anode

Calendar aging of lithium metal anodes (LMAs) is both ubiquitous and crucial in practical applications, representing an emerging and non-negligible issue. Herein, the controlled potential-holding method (CPHM) is performed to correlate solid–electrolyte interphase (SEI) formation protocols with calendar aging improvements. By identifying the distinctive decomposition potentials of anions and solvents in various electrolytes, holding the decomposition potential of anions promotes the preferential anion reduction to form the inorganic anion-derived SEI. Based on the electrochemical–mechanical model, the SEI formed via CPHM effectively prolongs the interface failure and facilitates uniform Li deposition, thereby mitigating the chemical corrosion during calendar aging. Furthermore, the synergistic effects of the stable SEI and uniform Li deposition benefit highly reversible Li plating/stripping, with a prolonged ∼70% longer lifespan after calendar aging. Overall, this study sheds light on improving calendar aging through regulating SEI formation, thereby paving the way for the practical adoption of LMAs.