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Title: Thermally driven mesoscale chemomechanical interplay in Li0.5Ni0.6Mn0.2Co0.2O2 cathode materials

Abstract

While Li ion batteries are intended to be operated within a mild temperature window, their structural and chemical complexity could lead to unanticipated local electrochemical events that could cause extreme temperature spikes, which, in turn, could trigger more undesired and sophisticated reactions in the system. Visualizing and understanding the response of battery electrode materials to thermal abuse conditions could potentially offer a knowledge basis for the prevention and mitigation of the safety hazards. Here we show a comprehensive investigation of thermally driven chemomechanical interplay in a Li0.5Ni0.6Mn0.2Co0.2O2 (charged NMC622) cathode material. We report that, at the early stage of the thermal abuse, oxygen release and internal Li migration occur concurrently, and are accompanied by mechanical disintegration at the mesoscale. At the later stage, Li protrusions are observed on the secondary particle surface due to the limited lithium solubility in non-layered lattices. As a result, the extraction of both oxygen and lithium from the host material at elevated temperature could influence the chemistry and safety at the cell level via rearrangement of the electron and ion diffusion pathways, reduction of the coulombic efficiency, and/or causing an internal short circuit that could provoke a thermal runaway.

Authors:
 [1];  [2];  [3];  [4];  [5];  [5];  [6];  [7];  [3];  [3]; ORCiD logo [8];  [9];  [10];  [3]; ORCiD logo [4]; ORCiD logo [3]
  1. Univ. of Science and Technology of China, Hefei (China); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  2. Tianjin Univ., Tianjin (China); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  4. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
  5. Stanford Univ., Stanford, CA (United States)
  6. European Synchrotron Radiation Facility, Grenoble (France)
  7. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  8. Tianjin Univ., Tianjin (China)
  9. Univ. of Science and Technology of China, Hefei (China)
  10. Purdue Univ., West Lafayette, LA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1490862
Grant/Contract Number:  
AC02-76SF00515; ECCS-1542152; DMR-1832613; DMR-1832707
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 6; Journal Issue: 45; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Wei, Chenxi, Zhang, Yan, Lee, Sang -Jun, Mu, Linqin, Liu, Jin, Wang, Chenxu, Yang, Yang, Doeff, Marca, Pianetta, Piero, Nordlund, Dennis, Du, Xi -Wen, Tian, Yangchao, Zhao, Kejie, Lee, Jun -Sik, Lin, Feng, and Liu, Yijin. Thermally driven mesoscale chemomechanical interplay in Li0.5Ni0.6Mn0.2Co0.2O2 cathode materials. United States: N. p., 2018. Web. https://doi.org/10.1039/c8ta08973f.
Wei, Chenxi, Zhang, Yan, Lee, Sang -Jun, Mu, Linqin, Liu, Jin, Wang, Chenxu, Yang, Yang, Doeff, Marca, Pianetta, Piero, Nordlund, Dennis, Du, Xi -Wen, Tian, Yangchao, Zhao, Kejie, Lee, Jun -Sik, Lin, Feng, & Liu, Yijin. Thermally driven mesoscale chemomechanical interplay in Li0.5Ni0.6Mn0.2Co0.2O2 cathode materials. United States. https://doi.org/10.1039/c8ta08973f
Wei, Chenxi, Zhang, Yan, Lee, Sang -Jun, Mu, Linqin, Liu, Jin, Wang, Chenxu, Yang, Yang, Doeff, Marca, Pianetta, Piero, Nordlund, Dennis, Du, Xi -Wen, Tian, Yangchao, Zhao, Kejie, Lee, Jun -Sik, Lin, Feng, and Liu, Yijin. Wed . "Thermally driven mesoscale chemomechanical interplay in Li0.5Ni0.6Mn0.2Co0.2O2 cathode materials". United States. https://doi.org/10.1039/c8ta08973f. https://www.osti.gov/servlets/purl/1490862.
@article{osti_1490862,
title = {Thermally driven mesoscale chemomechanical interplay in Li0.5Ni0.6Mn0.2Co0.2O2 cathode materials},
author = {Wei, Chenxi and Zhang, Yan and Lee, Sang -Jun and Mu, Linqin and Liu, Jin and Wang, Chenxu and Yang, Yang and Doeff, Marca and Pianetta, Piero and Nordlund, Dennis and Du, Xi -Wen and Tian, Yangchao and Zhao, Kejie and Lee, Jun -Sik and Lin, Feng and Liu, Yijin},
abstractNote = {While Li ion batteries are intended to be operated within a mild temperature window, their structural and chemical complexity could lead to unanticipated local electrochemical events that could cause extreme temperature spikes, which, in turn, could trigger more undesired and sophisticated reactions in the system. Visualizing and understanding the response of battery electrode materials to thermal abuse conditions could potentially offer a knowledge basis for the prevention and mitigation of the safety hazards. Here we show a comprehensive investigation of thermally driven chemomechanical interplay in a Li0.5Ni0.6Mn0.2Co0.2O2 (charged NMC622) cathode material. We report that, at the early stage of the thermal abuse, oxygen release and internal Li migration occur concurrently, and are accompanied by mechanical disintegration at the mesoscale. At the later stage, Li protrusions are observed on the secondary particle surface due to the limited lithium solubility in non-layered lattices. As a result, the extraction of both oxygen and lithium from the host material at elevated temperature could influence the chemistry and safety at the cell level via rearrangement of the electron and ion diffusion pathways, reduction of the coulombic efficiency, and/or causing an internal short circuit that could provoke a thermal runaway.},
doi = {10.1039/c8ta08973f},
journal = {Journal of Materials Chemistry. A},
number = 45,
volume = 6,
place = {United States},
year = {2018},
month = {10}
}

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Figures / Tables:

Fig. 1 Fig. 1 : Chemical evolution of a Li0.5Ni0.6Mn0.2Co0.2O2 secondary particle recorded using full-field X ray spectro-microscopy under the thermal abuse condition (380 °C). Panels a-d show the evolution in the 2D distribution of Ni valence state (color coded to the corresponding color map with red and blue indicating more oxidizedmore » and more reduced domains, respectively) as the particle is exposed to high temperature for different amount of time. Panels e-g show the differential valence maps between a and b, b and c, c and d, respectively. Panel h shows that the probability distribution of the Ni’s local valance state shifts toward lower energy upon heating. Panel i shows the probability distribution of the differential edge energy in panels e-g. The particle’s diameter is about 8 microns.« less

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      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.