Stable operation of rechargeable lithium-based batteries at low temperatures is important for cold-climate applications, but is plagued by dendritic Li plating and unstable solid–electrolyte interphase (SEI). Here, we report on high-performance Li metal batteries under low-temperature and high-rate-charging conditions. The high performance is achieved by using a self-assembled monolayer of electrochemically active molecules on current collectors that regulates the nanostructure and composition of the SEI and deposition morphology of Li metal anodes. A multilayer SEI that contains a lithium fluoride-rich inner phase and amorphous outer layer effectively seals the Li surface, in contrast to the conventional SEI, which is non-passive at low temperatures. Consequently, galvanic Li corrosion and self-discharge are suppressed, stable Li deposition is achieved from −60 °C to 45 °C, and a Li | LiCoO2 cell with a capacity of 2.0 mAh cm−2 displays a 200-cycle life at −15 °C with a recharge time of 45 min.
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This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the US Department of Energy, through the Advanced Battery Materials Research (BMR) Program (Battery500 Consortium) award no. DE-EE0008198. T.R. and A.T.N. acknowledge the provision of computing resources on Bebop, a high-performance computing cluster operated by the Laboratory Computing Resource Center at Argonne National Laboratory. We thank S. Zheng for discussion on the performance of batteries at low temperatures.
The authors declare no competing interests.
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Gao, Y., Rojas, T., Wang, K. et al. Low-temperature and high-rate-charging lithium metal batteries enabled by an electrochemically active monolayer-regulated interface. Nat Energy 5, 534–542 (2020). https://doi.org/10.1038/s41560-020-0640-7
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