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Title: X-ray nanotomography analysis of the microstructural evolution of LiMn2O4 electrodes

Abstract

One of the greatest challenges for advancing lithium-ion battery (LIB) technology is to minimize cell degradation during operation for long-term stability. To this end, it is important to understand how cell performance during operation relates to complex LIB microstructures. In this report, transmission X-ray microscopy (TXM) nanotomography is used to gain quantitative three-dimensional (3D) microstructure-performance correlations of LIB cathodes during cycling. The 3D microstructures of LiMn2O4 (LMO) electrodes, cycled under different conditions, including cycle number, operating voltage, and temperature, are characterized via TXM and statistically analyzed to investigate the impact of cycling conditions on the electrode microstructural evolution and cell performance. It is found that the number of cracks formed within LMO particles correlated with capacity fade. For the cell cycled at elevated temperatures, which exhibits the most severe capacity fade among all cells tested, mechanical cracking observed in TXM is not the only dominant contributor to the observed degradation. Mn2+ dissolution, as verified by detection of Mn on the counter electrode by energy dispersive spectrometry, also contributed. The current work demonstrate 3D TXM nanotomography as a powerful tool to help probe in-depth.

Authors:
 [1];  [2];  [3];  [4];  [5];  [4];  [1];  [1]
  1. Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
  2. Northwestern Univ., Evanston, IL (United States). Dept. of Chemical and Biological Engineering; Central South Univ., Changsha (China). College of Chemistry and Chemical Engineering
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II); Stony Brook Univ., NY (United States). Dept. of Materials Science and Chemical Engineering
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  5. Northwestern Univ., Evanston, IL (United States). Dept. of Chemical and Biological Engineering
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Electrical Energy Storage (CEES)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1436252
Alternate Identifier(s):
OSTI ID: 1550341
Report Number(s):
BNL-203494-2018-JAAM
Journal ID: ISSN 0378-7753
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Power Sources
Additional Journal Information:
Journal Volume: 360; Journal Issue: C; Journal ID: ISSN 0378-7753
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Liu, Zhao, Han, Kai, Chen-Wiegart, Yu-chen Karen, Wang, Jiajun, Kung, Harold H., Wang, Jun, Barnett, Scott A., and Faber, Katherine T.. X-ray nanotomography analysis of the microstructural evolution of LiMn2O4 electrodes. United States: N. p., 2017. Web. https://doi.org/10.1016/j.jpowsour.2017.06.027.
Liu, Zhao, Han, Kai, Chen-Wiegart, Yu-chen Karen, Wang, Jiajun, Kung, Harold H., Wang, Jun, Barnett, Scott A., & Faber, Katherine T.. X-ray nanotomography analysis of the microstructural evolution of LiMn2O4 electrodes. United States. https://doi.org/10.1016/j.jpowsour.2017.06.027
Liu, Zhao, Han, Kai, Chen-Wiegart, Yu-chen Karen, Wang, Jiajun, Kung, Harold H., Wang, Jun, Barnett, Scott A., and Faber, Katherine T.. Sat . "X-ray nanotomography analysis of the microstructural evolution of LiMn2O4 electrodes". United States. https://doi.org/10.1016/j.jpowsour.2017.06.027. https://www.osti.gov/servlets/purl/1436252.
@article{osti_1436252,
title = {X-ray nanotomography analysis of the microstructural evolution of LiMn2O4 electrodes},
author = {Liu, Zhao and Han, Kai and Chen-Wiegart, Yu-chen Karen and Wang, Jiajun and Kung, Harold H. and Wang, Jun and Barnett, Scott A. and Faber, Katherine T.},
abstractNote = {One of the greatest challenges for advancing lithium-ion battery (LIB) technology is to minimize cell degradation during operation for long-term stability. To this end, it is important to understand how cell performance during operation relates to complex LIB microstructures. In this report, transmission X-ray microscopy (TXM) nanotomography is used to gain quantitative three-dimensional (3D) microstructure-performance correlations of LIB cathodes during cycling. The 3D microstructures of LiMn2O4 (LMO) electrodes, cycled under different conditions, including cycle number, operating voltage, and temperature, are characterized via TXM and statistically analyzed to investigate the impact of cycling conditions on the electrode microstructural evolution and cell performance. It is found that the number of cracks formed within LMO particles correlated with capacity fade. For the cell cycled at elevated temperatures, which exhibits the most severe capacity fade among all cells tested, mechanical cracking observed in TXM is not the only dominant contributor to the observed degradation. Mn2+ dissolution, as verified by detection of Mn on the counter electrode by energy dispersive spectrometry, also contributed. The current work demonstrate 3D TXM nanotomography as a powerful tool to help probe in-depth.},
doi = {10.1016/j.jpowsour.2017.06.027},
journal = {Journal of Power Sources},
number = C,
volume = 360,
place = {United States},
year = {2017},
month = {6}
}

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    journal, August 2019


    A Physics-Based Model Capacity Fade Analysis of LiMn 2 O 4 /Graphite Cell at Different Temperatures
    journal, November 2018

    • Appiah, Williams Agyei; Ryou, Myung-Hyun; Lee, Yong Min
    • Journal of The Electrochemical Society, Vol. 166, Issue 3
    • DOI: 10.1149/2.0161903jes