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

Qianqian Li (), Zhenpeng Yao, Eungje Lee, Yaobin Xu, Michael M. Thackeray, Chris Wolverton, Vinayak P. Dravid () and Jinsong Wu ()
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Qianqian Li: Wuhan University of Technology
Zhenpeng Yao: Northwestern University
Eungje Lee: Argonne National Laboratory
Yaobin Xu: Northwestern University
Michael M. Thackeray: Argonne National Laboratory
Chris Wolverton: Northwestern University
Vinayak P. Dravid: Northwestern University
Jinsong Wu: Wuhan University of Technology

Nature Communications, 2019, vol. 10, issue 1, 1-7

Abstract: 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.

Date: 2019
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DOI: 10.1038/s41467-019-09408-2

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