Electrolyte design for Li-ion batteries under extreme operating conditions

Jijian Xu, Jiaxun Zhang, Travis P. Pollard, Qingdong Li, Sha Tan, Singyuk Hou, Hongli Wan, Fu Chen, Huixin He, Enyuan Hu, Kang Xu, Xiao-Qing Yang, Oleg Borodin () and Chunsheng Wang ()
Additional contact information
Jijian Xu: University of Maryland
Jiaxun Zhang: University of Maryland
Travis P. Pollard: US DEVCOM Army Research Laboratory
Qingdong Li: The State University of New Jersey
Sha Tan: Brookhaven National Laboratory
Singyuk Hou: University of Maryland
Hongli Wan: University of Maryland
Fu Chen: University of Maryland
Huixin He: The State University of New Jersey
Enyuan Hu: Brookhaven National Laboratory
Kang Xu: US DEVCOM Army Research Laboratory
Xiao-Qing Yang: Brookhaven National Laboratory
Oleg Borodin: US DEVCOM Army Research Laboratory
Chunsheng Wang: University of Maryland

Nature, 2023, vol. 614, issue 7949, 694-700

Abstract: Abstract The ideal electrolyte for the widely used LiNi0.8Mn0.1Co0.1O2 (NMC811)||graphite lithium-ion batteries is expected to have the capability of supporting higher voltages (≥4.5 volts), fast charging (≤15 minutes), charging/discharging over a wide temperature range (±60 degrees Celsius) without lithium plating, and non-flammability1–4. No existing electrolyte simultaneously meets all these requirements and electrolyte design is hindered by the absence of an effective guiding principle that addresses the relationships between battery performance, solvation structure and solid-electrolyte-interphase chemistry5. Here we report and validate an electrolyte design strategy based on a group of soft solvents that strikes a balance between weak Li+–solvent interactions, sufficient salt dissociation and desired electrochemistry to fulfil all the aforementioned requirements. Remarkably, the 4.5-volt NMC811||graphite coin cells with areal capacities of more than 2.5 milliampere hours per square centimetre retain 75 per cent (54 per cent) of their room-temperature capacity when these cells are charged and discharged at −50 degrees Celsius (−60 degrees Celsius) at a C rate of 0.1C, and the NMC811||graphite pouch cells with lean electrolyte (2.5 grams per ampere hour) achieve stable cycling with an average Coulombic efficiency of more than 99.9 per cent at −30 degrees Celsius. The comprehensive analysis further reveals an impedance matching between the NMC811 cathode and the graphite anode owing to the formation of similar lithium-fluoride-rich interphases, thus effectively avoiding lithium plating at low temperatures. This electrolyte design principle can be extended to other alkali-metal-ion batteries operating under extreme conditions.

Date: 2023
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DOI: 10.1038/s41586-022-05627-8

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