skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Dynamic imaging of crystalline defects in lithium-manganese oxide electrodes during electrochemical activation to high voltage

Abstract

Crystalline defects are commonly generated in lithium-metal-oxide electrodes during cycling of lithium-ion batteries. Their role in electrochemical reactions is not yet fully understood because, until recently, there has not been an effective operando technique to image dynamic processes at the atomic level. In this study, two types of defects were monitored dynamically during delithiation and concomitant oxidation of oxygen ions by using in situ high-resolution transmission electron microscopy supported by density functional theory calculations. One stacking fault with a fault vector b/6[110] and low mobility contributes minimally to oxygen release from the structure. In contrast, dissociated dislocations with Burgers vector of c/2[001] have high gliding and transverse mobility; they lead to the formation, transport and release subsequently of oxygen related species at the surface of the electrode particles. This work advances the scientific understanding of how oxygen participates and the structural response during the activation process at high potentials.

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [4];  [3];  [4];  [4];  [5]
  1. Wuhan Univ. of Technology, Hubei (China); Shanghai Univ., Shanghai (China); Northwestern Univ., Evanston, IL (United States)
  2. Northwestern Univ., Evanston, IL (United States); Harvard Univ., Cambridge, MA (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Northwestern Univ., Evanston, IL (United States)
  5. Wuhan Univ. of Technology, Hubei (China); Northwestern Univ., Evanston, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1510310
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Li, Qianqian, Yao, Zhenpeng, Lee, Eungje, Xu, Yaobin, Thackeray, Michael M., Wolverton, Chris, Dravid, Vinayak P., and Wu, Jinsong. Dynamic imaging of crystalline defects in lithium-manganese oxide electrodes during electrochemical activation to high voltage. United States: N. p., 2019. Web. doi:10.1038/s41467-019-09408-2.
Li, Qianqian, Yao, Zhenpeng, Lee, Eungje, Xu, Yaobin, Thackeray, Michael M., Wolverton, Chris, Dravid, Vinayak P., & Wu, Jinsong. Dynamic imaging of crystalline defects in lithium-manganese oxide electrodes during electrochemical activation to high voltage. United States. doi:10.1038/s41467-019-09408-2.
Li, Qianqian, Yao, Zhenpeng, Lee, Eungje, Xu, Yaobin, Thackeray, Michael M., Wolverton, Chris, Dravid, Vinayak P., and Wu, Jinsong. Fri . "Dynamic imaging of crystalline defects in lithium-manganese oxide electrodes during electrochemical activation to high voltage". United States. doi:10.1038/s41467-019-09408-2. https://www.osti.gov/servlets/purl/1510310.
@article{osti_1510310,
title = {Dynamic imaging of crystalline defects in lithium-manganese oxide electrodes during electrochemical activation to high voltage},
author = {Li, Qianqian and Yao, Zhenpeng and Lee, Eungje and Xu, Yaobin and Thackeray, Michael M. and Wolverton, Chris and Dravid, Vinayak P. and Wu, Jinsong},
abstractNote = {Crystalline defects are commonly generated in lithium-metal-oxide electrodes during cycling of lithium-ion batteries. Their role in electrochemical reactions is not yet fully understood because, until recently, there has not been an effective operando technique to image dynamic processes at the atomic level. In this study, two types of defects were monitored dynamically during delithiation and concomitant oxidation of oxygen ions by using in situ high-resolution transmission electron microscopy supported by density functional theory calculations. One stacking fault with a fault vector b/6[110] and low mobility contributes minimally to oxygen release from the structure. In contrast, dissociated dislocations with Burgers vector of c/2[001] have high gliding and transverse mobility; they lead to the formation, transport and release subsequently of oxygen related species at the surface of the electrode particles. This work advances the scientific understanding of how oxygen participates and the structural response during the activation process at high potentials.},
doi = {10.1038/s41467-019-09408-2},
journal = {Nature Communications},
issn = {2041-1723},
number = 1,
volume = 10,
place = {United States},
year = {2019},
month = {4}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Save / Share:

Works referenced in this record:

Improved capacity retention in rechargeable 4 V lithium/lithium-manganese oxide (spinel) cells
journal, April 1994


In Situ Observation of the Electrochemical Lithiation of a Single SnO2 Nanowire Electrode
journal, December 2010


High-resolution X-ray diffraction, DIFFaX, NMR and first principles study of disorder in the Li2MnO3�Li[Ni1/2Mn1/2]O2 solid solution
journal, September 2005

  • Br�ger, Julien; Jiang, Meng; Dupr�, Nicolas
  • Journal of Solid State Chemistry, Vol. 178, Issue 9, p. 2575-2585
  • DOI: 10.1016/j.jssc.2005.05.027

Phospho-olivines as Positive-Electrode Materials for Rechargeable Lithium Batteries
journal, April 1997

  • Padhi, A. K.
  • Journal of The Electrochemical Society, Vol. 144, Issue 4, p. 1188-1194
  • DOI: 10.1149/1.1837571