Ultra-Low Temperature Li/CFx Batteries Enabled by Fast-transport and Anion-pairing Liquefied Gas Electrolytes

Lithium fluorinated carbon is one of the most promising chemistries for high-energy-density primary energy storage systems in applications where rechargeability is not required. Though Li/CFx demonstrates high energy density under ambient conditions, achieving such a high energy density when exposed to subzero temperatures remains a challenge, particularly under high current density. Here, we report a liquefied gas electrolyte with an anion-pair solvation structure based on dimethyl ether with a low melting point and low viscosity, leading to high ionic conductivity between a wide temperature range. Besides that, through systematic X-ray photoelectron spectroscopy integrated with transmission electron microscopy characterizations, we evaluate the interface of CFx for low-temperature performance. We conclude that the fast transport and anion-pairing solvation structure of the electrolyte bring about reduced charge transfer resistance at low temperatures, which resulted in significantly enhanced performance of Li/CFx cells. Utilizing 50 mg/cm2 loading electrodes, the Li/CFx still displayed 1530 Wh/kg at reduced temperature. This work provides insights into the electrolyte design that may overcome the operational limits of batteries in extreme environments.