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Title: Electrolyte design for Li-ion batteries under extreme operating conditions

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-flammability. 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 chemistry. 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 themore » NMC811 cathode and the graphite anode owing to the formation of similar lithium-fluoride-rich interphases, thus effectively avoiding lithium plating at low temperatures. Additionally, this electrolyte design principle can be extended to other alkali-metal-ion batteries operating under extreme conditions.« less

Authors:
ORCiD logo [1];  [1]; ORCiD logo [2];  [3]; ORCiD logo [4];  [1];  [1];  [1];  [3]; ORCiD logo [4]; ORCiD logo [2]; ORCiD logo [4]; ORCiD logo [2]; ORCiD logo [1]
  1. University of Maryland, College Park, MD (United States)
  2. Army Research Laboratory, Adelphi, MD (United States)
  3. Rutgers University, New Brunswick, NJ (United States)
  4. Brookhaven National Laboratory (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; US Army Research Laboratory (USARL)
OSTI Identifier:
1924195
Report Number(s):
BNL-224007-2023-JAAM
Journal ID: ISSN 0028-0836
Grant/Contract Number:  
SC0012704; W911NF-20-2-0284
Resource Type:
Accepted Manuscript
Journal Name:
Nature (London)
Additional Journal Information:
Journal Name: Nature (London); Journal Volume: 614; Journal Issue: 7949; Journal ID: ISSN 0028-0836
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; electrolyte; low temperature; high voltage; lithium-ion battery

Citation Formats

Xu, Jijian, Zhang, Jiaxun, Pollard, Travis P., Li, Qingdong, Tan, Sha, Hou, Singyuk, Wan, Hongli, Chen, Fu, He, Huixin, Hu, Enyuan, Xu, Kang, Yang, Xiao-Qing, Borodin, Oleg, and Wang, Chunsheng. Electrolyte design for Li-ion batteries under extreme operating conditions. United States: N. p., 2023. Web. doi:10.1038/s41586-022-05627-8.
Xu, Jijian, Zhang, Jiaxun, Pollard, Travis P., Li, Qingdong, Tan, Sha, Hou, Singyuk, Wan, Hongli, Chen, Fu, He, Huixin, Hu, Enyuan, Xu, Kang, Yang, Xiao-Qing, Borodin, Oleg, & Wang, Chunsheng. Electrolyte design for Li-ion batteries under extreme operating conditions. United States. https://doi.org/10.1038/s41586-022-05627-8
Xu, Jijian, Zhang, Jiaxun, Pollard, Travis P., Li, Qingdong, Tan, Sha, Hou, Singyuk, Wan, Hongli, Chen, Fu, He, Huixin, Hu, Enyuan, Xu, Kang, Yang, Xiao-Qing, Borodin, Oleg, and Wang, Chunsheng. Wed . "Electrolyte design for Li-ion batteries under extreme operating conditions". United States. https://doi.org/10.1038/s41586-022-05627-8. https://www.osti.gov/servlets/purl/1924195.
@article{osti_1924195,
title = {Electrolyte design for Li-ion batteries under extreme operating conditions},
author = {Xu, Jijian and Zhang, Jiaxun and Pollard, Travis P. and Li, Qingdong and Tan, Sha and Hou, Singyuk and Wan, Hongli and Chen, Fu and He, Huixin and Hu, Enyuan and Xu, Kang and Yang, Xiao-Qing and Borodin, Oleg and Wang, Chunsheng},
abstractNote = {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-flammability. 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 chemistry. 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. Additionally, this electrolyte design principle can be extended to other alkali-metal-ion batteries operating under extreme conditions.},
doi = {10.1038/s41586-022-05627-8},
journal = {Nature (London)},
number = 7949,
volume = 614,
place = {United States},
year = {Wed Feb 08 00:00:00 EST 2023},
month = {Wed Feb 08 00:00:00 EST 2023}
}

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