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Title: Unlocking the self-supported thermal runaway of high-energy lithium-ion batteries

Abstract

Layered Ni-rich LiNixMnyCo1-x-yO2 (NMC) materials are the most promising cathode materials for Li-ion batteries due to their favorable energy densities. However, the low thermal stability typically caused by detrimental oxygen release leads to significant safety concerns. Determining the pathways of oxygen evolution reaction is essential, as the ideal safety countermeasure is to break the reaction chain of thermal runaway. In this study, we demonstrate that two endogenous pathways of oxygen involved in strong exothermic reactions lead the NMC811|graphite pouch cell to an uncontrollable state, and we quantify the individual contribution of the pathways to thermal runaway. Approximately 41% of thermal-induced oxygen reacts aggressively with ethylene carbonate (EC) at the cathode/electrolyte interface with 16% heat generation, accelerating the self-heating rate and thereby further triggering thermal runaway. The residual oxygen that survives the reaction with carbonate spreads to the lithiated anode with major heat generation (65%), bringing the battery to the maximum destructive temperature during thermal runaway. By confirming the significant roles of EC and anode, a deeper understanding on battery fire was achieved. Finally, the revealed mechanism can help guide studies on stopping the two reaction pathways, allowing for the safer use of high-energy lithium-ion batteries in the future.

Authors:
 [1];  [1];  [1];  [2];  [3];  [1];  [1];  [1];  [1];  [1];  [1];  [4];  [5];  [6];  [2];  [7];  [1];  [1];  [3];  [1]
  1. Tsinghua Univ., Beijing (China)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Nissan Motor Co., Ltd., Yokosuka (Japan)
  4. R&D China, Électricité de France, Beijing (China)
  5. Think Energy Co., Ltd., Beijing (China)
  6. Tsinghua Univ., Beijing (China); Think Energy Co., Ltd., Beijing (China)
  7. Argonne National Lab. (ANL), Argonne, IL (United States); Stanford Univ., CA (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; Ministry of Science and Technology of the Republic of China (MOST); National Natural Science Foundation of China (NSFC); China Postdoctoral Science Foundation; Tsinghua University; U.S.-China Clean Energy Research Center (CERC)
OSTI Identifier:
1820567
Grant/Contract Number:  
AC02-06CH11357; 2019YFE0100200; 52006115; 52076121; BX20190162; 2019M660631; 2019Z02UTY06
Resource Type:
Accepted Manuscript
Journal Name:
Energy Storage Materials
Additional Journal Information:
Journal Volume: 39; Journal ID: ISSN 2405-8297
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Hou, Junxian, Feng, Xuning, Wang, Li, Liu, Xiang, Ohma, Atsushi, Lu, Languang, Ren, Dongsheng, Huang, Wensheng, Li, Yan, Yi, Mengchao, Wang, Yu, Ren, Jianqiao, Meng, Zihan, Chu, Zhengyu, Xu, Gui-Liang, Amine, Khalil, He, Xiangming, Wang, Hewu, Nitta, Yoshiaki, and Ouyang, Minggao. Unlocking the self-supported thermal runaway of high-energy lithium-ion batteries. United States: N. p., 2021. Web. doi:10.1016/j.ensm.2021.04.035.
Hou, Junxian, Feng, Xuning, Wang, Li, Liu, Xiang, Ohma, Atsushi, Lu, Languang, Ren, Dongsheng, Huang, Wensheng, Li, Yan, Yi, Mengchao, Wang, Yu, Ren, Jianqiao, Meng, Zihan, Chu, Zhengyu, Xu, Gui-Liang, Amine, Khalil, He, Xiangming, Wang, Hewu, Nitta, Yoshiaki, & Ouyang, Minggao. Unlocking the self-supported thermal runaway of high-energy lithium-ion batteries. United States. https://doi.org/10.1016/j.ensm.2021.04.035
Hou, Junxian, Feng, Xuning, Wang, Li, Liu, Xiang, Ohma, Atsushi, Lu, Languang, Ren, Dongsheng, Huang, Wensheng, Li, Yan, Yi, Mengchao, Wang, Yu, Ren, Jianqiao, Meng, Zihan, Chu, Zhengyu, Xu, Gui-Liang, Amine, Khalil, He, Xiangming, Wang, Hewu, Nitta, Yoshiaki, and Ouyang, Minggao. Fri . "Unlocking the self-supported thermal runaway of high-energy lithium-ion batteries". United States. https://doi.org/10.1016/j.ensm.2021.04.035. https://www.osti.gov/servlets/purl/1820567.
@article{osti_1820567,
title = {Unlocking the self-supported thermal runaway of high-energy lithium-ion batteries},
author = {Hou, Junxian and Feng, Xuning and Wang, Li and Liu, Xiang and Ohma, Atsushi and Lu, Languang and Ren, Dongsheng and Huang, Wensheng and Li, Yan and Yi, Mengchao and Wang, Yu and Ren, Jianqiao and Meng, Zihan and Chu, Zhengyu and Xu, Gui-Liang and Amine, Khalil and He, Xiangming and Wang, Hewu and Nitta, Yoshiaki and Ouyang, Minggao},
abstractNote = {Layered Ni-rich LiNixMnyCo1-x-yO2 (NMC) materials are the most promising cathode materials for Li-ion batteries due to their favorable energy densities. However, the low thermal stability typically caused by detrimental oxygen release leads to significant safety concerns. Determining the pathways of oxygen evolution reaction is essential, as the ideal safety countermeasure is to break the reaction chain of thermal runaway. In this study, we demonstrate that two endogenous pathways of oxygen involved in strong exothermic reactions lead the NMC811|graphite pouch cell to an uncontrollable state, and we quantify the individual contribution of the pathways to thermal runaway. Approximately 41% of thermal-induced oxygen reacts aggressively with ethylene carbonate (EC) at the cathode/electrolyte interface with 16% heat generation, accelerating the self-heating rate and thereby further triggering thermal runaway. The residual oxygen that survives the reaction with carbonate spreads to the lithiated anode with major heat generation (65%), bringing the battery to the maximum destructive temperature during thermal runaway. By confirming the significant roles of EC and anode, a deeper understanding on battery fire was achieved. Finally, the revealed mechanism can help guide studies on stopping the two reaction pathways, allowing for the safer use of high-energy lithium-ion batteries in the future.},
doi = {10.1016/j.ensm.2021.04.035},
journal = {Energy Storage Materials},
number = ,
volume = 39,
place = {United States},
year = {Fri Apr 30 00:00:00 EDT 2021},
month = {Fri Apr 30 00:00:00 EDT 2021}
}

Works referenced in this record:

Designing an intrinsically safe organic electrolyte for rechargeable batteries
journal, October 2020


Revealing the multilevel thermal safety of lithium batteries
journal, October 2020


Recent advances of thermal safety of lithium ion battery for energy storage
journal, October 2020


Thermal Runaway of Lithium-Ion Batteries without Internal Short Circuit
journal, October 2018


Oxygen Release Degradation in Li‐Ion Battery Cathode Materials: Mechanisms and Mitigating Approaches
journal, April 2019

  • Sharifi‐Asl, Soroosh; Lu, Jun; Amine, Khalil
  • Advanced Energy Materials, Vol. 9, Issue 22
  • DOI: 10.1002/aenm.201900551

Superconcentrated electrolytes for a high-voltage lithium-ion battery
journal, June 2016

  • Wang, Jianhui; Yamada, Yuki; Sodeyama, Keitaro
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms12032

Spinel materials for Li-ion batteries: new insights obtained by operando neutron and synchrotron X-ray diffraction
journal, November 2015

  • Bianchini, Matteo; Fauth, François; Suard, Emmanuelle
  • Acta Crystallographica Section B Structural Science, Crystal Engineering and Materials, Vol. 71, Issue 6
  • DOI: 10.1107/S2052520615017199

Singlet oxygen evolution from layered transition metal oxide cathode materials and its implications for lithium-ion batteries
journal, October 2018


Thermal runaway of Lithium-ion batteries employing LiN(SO2F)2-based concentrated electrolytes
journal, October 2020


Mitigating Thermal Runaway of Lithium-Ion Batteries
journal, April 2020


Thermally-driven mesopore formation and oxygen release in delithiated NCA cathode particles
journal, January 2019

  • Besli, Münir M.; Shukla, Alpesh Khushalchand; Wei, Chenxi
  • Journal of Materials Chemistry A, Vol. 7, Issue 20
  • DOI: 10.1039/C9TA01720H

Model-based thermal runaway prediction of lithium-ion batteries from kinetics analysis of cell components
journal, October 2018


A reliable approach of differentiating discrete sampled-data for battery diagnosis
journal, February 2020


Revealing electrolyte oxidation via carbonate dehydrogenation on Ni-based oxides in Li-ion batteries by in situ Fourier transform infrared spectroscopy
journal, January 2020

  • Zhang, Yirui; Katayama, Yu; Tatara, Ryoichi
  • Energy & Environmental Science, Vol. 13, Issue 1
  • DOI: 10.1039/C9EE02543J

Fire-extinguishing organic electrolytes for safe batteries
journal, November 2017


The Thermal Stability of Lithium Solid Electrolytes with Metallic Lithium
journal, April 2020


Theoretical Study of Li Migration in Lithium–Graphite Intercalation Compounds with Dispersion-Corrected DFT Methods
journal, January 2014

  • Thinius, Sascha; Islam, Mazharul M.; Heitjans, Paul
  • The Journal of Physical Chemistry C, Vol. 118, Issue 5
  • DOI: 10.1021/jp408945j

Thermal runaway mechanism of lithium ion battery for electric vehicles: A review
journal, January 2018


A Long Cycle‐Life High‐Voltage Spinel Lithium‐Ion Battery Electrode Achieved by Site‐Selective Doping
journal, April 2020

  • Liang, Gemeng; Wu, Zhibin; Didier, Christophe
  • Angewandte Chemie International Edition, Vol. 59, Issue 26
  • DOI: 10.1002/anie.202001454

High-nickel layered oxide cathodes for lithium-based automotive batteries
journal, January 2020


Probing the Thermal-Driven Structural and Chemical Degradation of Ni-Rich Layered Cathodes by Co/Mn Exchange
journal, November 2020

  • Liu, Xiang; Xu, Gui-Liang; Yin, Liang
  • Journal of the American Chemical Society, Vol. 142, Issue 46
  • DOI: 10.1021/jacs.0c09961

A review on lithium combustion
journal, January 2016


Effect of Heat Treatment on Si Electrodes Using Polyvinylidene Fluoride Binder
journal, January 2008

  • Li, Jing; Christensen, L.; Obrovac, M. N.
  • Journal of The Electrochemical Society, Vol. 155, Issue 3
  • DOI: 10.1149/1.2830545

Thermal stress-induced charge and structure heterogeneity in emerging cathode materials
journal, May 2020


Thermal Runaway Triggered by Plated Lithium on the Anode after Fast Charging
journal, November 2019

  • Li, Yalun; Feng, Xuning; Ren, Dongsheng
  • ACS Applied Materials & Interfaces, Vol. 11, Issue 50
  • DOI: 10.1021/acsami.9b16589

A comparative investigation of aging effects on thermal runaway behavior of lithium-ion batteries
journal, November 2019


Quantitative identification of emissions from abused prismatic Ni-rich lithium-ion batteries
journal, November 2019


Lithium-Ion Battery Supply Chain Considerations: Analysis of Potential Bottlenecks in Critical Metals
journal, October 2017


New Concepts in Electrolytes
journal, February 2020


Thermal analysis of nickel cobalt lithium manganese with varying nickel content used for lithium ion batteries
journal, September 2017


Non-flammable electrolytes with high salt-to-solvent ratios for Li-ion and Li-metal batteries
journal, July 2018


A review on the key issues of the lithium ion battery degradation among the whole life cycle
journal, August 2019


Thermal runaway caused fire and explosion of lithium ion battery
journal, June 2012


Oxygen Release and Its Effect on the Cycling Stability of LiNi x Mn y Co z O 2 (NMC) Cathode Materials for Li-Ion Batteries
journal, January 2017

  • Jung, Roland; Metzger, Michael; Maglia, Filippo
  • Journal of The Electrochemical Society, Vol. 164, Issue 7
  • DOI: 10.1149/2.0021707jes

A Review of Battery Fires in Electric Vehicles
journal, January 2020


Nonflammable organic electrolytes for high-safety lithium-ion batteries
journal, November 2020


Problems and their origins of Ni-rich layered oxide cathode materials
journal, January 2020


Investigating the thermal runaway mechanisms of lithium-ion batteries based on thermal analysis database
journal, July 2019


Pentaglyme–K salt binary mixtures: phase behavior, solvate structures, and physicochemical properties
journal, January 2015

  • Mandai, Toshihiko; Tsuzuki, Seiji; Ueno, Kazuhide
  • Physical Chemistry Chemical Physics, Vol. 17, Issue 4
  • DOI: 10.1039/C4CP05017G

Structural Changes and Thermal Stability of Charged LiNi x Mn y Co z O 2 Cathode Materials Studied by Combined In Situ Time-Resolved XRD and Mass Spectroscopy
journal, December 2014

  • Bak, Seong-Min; Hu, Enyuan; Zhou, Yongning
  • ACS Applied Materials & Interfaces, Vol. 6, Issue 24
  • DOI: 10.1021/am506712c