Lithium-ion batteries, known for their high energy density and long cycle life, have been widely used in portable electronics, electric vehicles, and energy storage systems. However, under extremely cold conditions, traditional lithium-ion batteries experience a drastic decline in both capacity and power output, while the risk of lithium dendrite formation during charging increases. These issues mainly stem from the increased viscosity of liquid electrolytes, elevated interfacial impedance, and reduced ionic conductivity, all of which severely hinder electrochemical kinetics and overall performance. In contrast, all-solid-state batteries (ASSBs) use solid-state electrolytes that are largely immune to temperature fluctuations. They eliminate the dissolution and desolvation limitations associated with liquid electrolytes at low temperatures, maintaining stable interfacial behavior and efficient ion transport. Furthermore, since ASSBs do not involve the liquid/solid desolvation process present in conventional batteries, they exhibit lower charge-transfer resistance and faster electrochemical reactions even under extremely cold conditions. Nonetheless, ASSBs still face challenges: grain boundary ion transport remains highly temperature-dependent, leading to reduced overall ionic conductivity at low temperatures. To overcome this, amorphous solid-state electrolytes have emerged as a promising solution — by eliminating grain boundaries, they provide isotropic ion transport pathways, thereby minimizing discontinuities in ion conduction and enhancing low-temperature battery performance.
Recently, the research team led by Professor Ruqiang Zou and Associate Professor Lei Gao from the SAM, Peking University Shenzhen Graduate School, in collaboration with Southern University of Science and Technology, published a paper in Nature Communications titled “All-solid-state batteries designed for operation under extreme cold conditions” (https://www.nature.com/articles/s41467-024-55154-5). The study reports the development of a novel amorphous solid electrolyte, xLi3N–TaCl5 (1 ≤ 3x ≤ 2), specifically engineered for operation in extreme cold environments, and the design of all-solid-state batteries based on this material. The optimized composition, L1.25NTCl (3x = 1.25), achieves a high ionic conductivity of 5.91 mS·cm⁻1 at 25 °C, ensuring efficient lithium-ion transport both in the bulk and across the cathode/electrolyte interface.
By integrating LiCoO2 (LCO) as the cathode, L1.25NTCl as the amorphous solid-state electrolyte, Li10GeP2S12 (LGPS) as an interfacial layer, and Li–In alloy as the anode, the team successfully designed an ASSB structure tailored for low-temperature operation. The resulting Li–In|LGPS–L1.25NTCl|LCO battery delivered outstanding performance, achieving discharge capacities of 183.19, 164.8, and 143.78 mAh·g⁻1 at –10 °C, –30 °C, and –40 °C, respectively. Even after 100 cycles at –30 °C and a current density of 18 mA·g⁻¹, the cell maintained 137.6 mAh·g⁻1 (capacity retention of 83.5%). Remarkably, the battery sustained over 200 hours of charge–discharge cycling at –60 °C, demonstrating its exceptional applicability in extreme cold environments.
The corresponding authors of the paper are Professor Ruqiang Zou, Associate Professor Lei Gao (Peking University Shenzhen Graduate School), and Professors Jinlong Zhu and Songbai Han (Southern University of Science and Technology). The first authors are doctoral candidate Bolong Hong and Associate Professor Lei Gao. Associate Professor Jiaxin Zheng and doctoral student Genming Lai from the SAM also made significant contributions to the theoretical modeling and calculations. This research was supported by the National Natural Science Foundation of China, the National Key Research and Development Program, and the Shenzhen Science and Technology Innovation Commission, among other funding sources.
