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Investigation of electrode-electrolyte interfaces to enable non-flammable Li-ion batteries operating up to 125°C with liquid electrolyte

Journal Article · · Cell Reports Physical Science
 [1];  [2];  [3];  [3];  [4];  [5];  [1]
  1. Wayne State Univ., Detroit, MI (United States)
  2. Brookhaven National Laboratory (BNL), Upton, NY (United States)
  3. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
  4. Canadian Light Source, Saskatoon, SK (Canada)
  5. Argonne National Laboratory (ANL), Argonne, IL (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
+ Show Author Affiliations
Non-flammable and high-temperature stable ionic liquid (IL)-based electrolytes could eliminate catastrophic battery failures and improve battery safety, but their poor electrochemical interaction with the LiNixMnyCozO2 (NMC) family of cathodes is a long-standing problem due to severe parasitic reactions at high temperature. Understanding surface and bulk structural mechanisms of NMC-type cathodes at elevated operational temperature is of paramount importance to facilitate stable electrochemical performance. Here, we report a non-flammable phosphonium IL-based cell chemistry that offers stable electrode-electrolyte interfaces, leading to electrochemical performance up to 125°C and high-temperature safety. We combine electrochemistry with multimodal X-ray spectroscopy methods to understand interfaces at elevated temperature (100°C). This nanoscale understating enables a proof-of-concept high-temperature cylindrical cell (14500), and the design achieves an average Coulombic efficiency of ≈99.5% up to 300 cycles at 100°C. The results ascertain the significance of depth-dependent degradation at the interface, guiding room-temperature Li-ion technology toward extreme-temperature applications.
Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Sponsoring Organization:
Advanced Energy Consortium (AEC); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC02-06CH11357; SC0012704
OSTI ID:
2570116
Report Number(s):
BNL--228312-2025-JAAM
Journal Information:
Cell Reports Physical Science, Journal Name: Cell Reports Physical Science Journal Issue: 5 Vol. 6; ISSN 2666-3864
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

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Figures / Tables (8)

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Related Subjects

36 MATERIALS SCIENCE
Li-ion batteries
X-ray absorption spectroscopy
cathode electrolyte interphase
electrode-electrolyte interface
environmental safety
high-temperature batteries
ionic liquid electrolytes
non-flammability