Regulation of Interfacial Chemistry Enabling High‐Power Dual‐Ion Batteries at Low Temperatures

Abstract Interfacial chemistry plays a crucial role in determining the electrochemical properties of low‐temperature rechargeable batteries. Although existing interface engineering has significantly improved the capacity of rechargeable batteries operating at low temperatures, challenges such as sharp voltage drops and poor high‐rate discharge capabilities continue to limit their applications in extreme environments. In this study, an energy‐level‐adaptive design strategy for electrolytes to regulate interfacial chemistry in low‐temperature Li||graphite dual‐ion batteries (DIBs) is proposed. This strategy enables the construction of robust interphases with superior ion‐transfer kinetics. On the graphite cathode, the design endues the cathode interface with solvent/anion‐coupled interfacial chemistry, which yields an nitrogen/phosphor/sulfur/fluorin (N/P/S/F)‐containing organic‐rich interphase to boost anion‐transfer kinetics and maintains excellent interfacial stability. On the Li metal anode, the anion‐derived interfacial chemistry promotes the formation of an inorganic‐dominant LiF‐rich interphase, which effectively suppresses Li dendrite growth and improves the Li plating/stripping kinetics at low temperatures. Consequently, the DIBs can operate within a wide temperature range, spanning from −40 to 45 °C. At −40 °C, the DIB exhibits exceptional performance, delivering 97.4% of its room‐temperature capacity at 1 C and displaying an extraordinarily high‐rate discharge capability with 62.3% capacity retention at 10 C. This study demonstrates a feasible strategy for the development of high‐power and low‐temperature rechargeable batteries.