Electrolyte Design for Low-Temperature Li-Metal Batteries: Challenges and Prospects

Highlights A critical assessment of electrolytes’ limiting factors, which affect the low-temperature performance of Li-metal batteries. Summary of emerging strategies to improve low-temperature performance from the aspects of electrolyte design and electrolyte/electrode interphase engineering. Perspectives and challenges on how to develop creative solutions in electrolytes and correlative materials for low-temperature operation. Electrolyte design holds the greatest opportunity for the development of batteries that are capable of sub-zero temperature operation. To get the most energy storage out of the battery at low temperatures, improvements in electrolyte chemistry need to be coupled with optimized electrode materials and tailored electrolyte/electrode interphases. Herein, this review critically outlines electrolytes’ limiting factors, including reduced ionic conductivity, large de-solvation energy, sluggish charge transfer, and slow Li-ion transportation across the electrolyte/electrode interphases, which affect the low-temperature performance of Li-metal batteries. Detailed theoretical derivations that explain the explicit influence of temperature on battery performance are presented to deepen understanding. Emerging improvement strategies from the aspects of electrolyte design and electrolyte/electrode interphase engineering are summarized and rigorously compared. Perspectives on future research are proposed to guide the ongoing exploration for better low-temperature Li-metal batteries.