Lithium metal batteries hold promise for pushing cell-level energy densities beyond 300 Wh kg−1 while operating at ultra-low temperatures (below −30 °C). Batteries capable of both charging and discharging at these temperature extremes are highly desirable due to their inherent reduction in the need for external warming. Here we demonstrate that the local solvation structure of the electrolyte defines the charge-transfer behaviour at ultra-low temperature, which is crucial for achieving high Li metal Coulombic efficiency and avoiding dendritic growth. These insights were applied to Li metal full-cells, where a high-loading 3.5 mAh cm−2 sulfurized polyacrylonitrile (SPAN) cathode was paired with a onefold excess Li metal anode. The cell retained 84% and 76% of its room temperature capacity when cycled at −40 and −60 °C, respectively, which presented stable performance over 50 cycles. This work provides design criteria for ultra-low-temperature lithium metal battery electrolytes, and represents a defining step for the performance of low-temperature batteries.
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This work was supported by a NASA Space Technology Graduate Research Opportunity. This work was also partially supported by the Office of Vehicle Technologies of the US Department of Energy through the Advanced Battery Materials Research (BMR) Program (Battery500 Consortium) under contract no. DE-EE0007764 to P.L. This work was also partially supported by an Early Career Faculty grant from NASA’s Space Technology Research Grants Program (ECF 80NSSC18K1512) to Z.C. Part of the work used the UCSD-MTI Battery Fabrication Facility and the UCSD-Arbin Battery Testing Facility. Electron microscopic characterization was performed at the San Diego Nanotechnology Infrastructure (SDNI) of UCSD, a member of the National Nanotechnology Coordinated Infrastructure, which is supported by the National Science Foundation (grant ECCS-1542148). Computational support for this work was provided by the National Energy Research Scientific Computing Center (NERSC), a US Department of Energy Office of Science User Facility operated under contract no. DE-AC02-05CH11231. This work also used the Extreme Science and Engineering Discovery Environment (XSEDE)53 on the Comet supercomputer at the San Diego Supercomputing Center, which is supported by National Science Foundation grant no. ACI-1548562.
The authors declare no competing interests.
Peer review information Nature Energy thanks Kevin Leung and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
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Holoubek, J., Liu, H., Wu, Z. et al. Tailoring electrolyte solvation for Li metal batteries cycled at ultra-low temperature. Nat Energy 6, 303–313 (2021). https://doi.org/10.1038/s41560-021-00783-z
Nature Energy (2021)