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

Li, Qianqian; Yao, Zhenpeng; Lee, Eungje; Xu, Yaobin; Thackeray, Michael M.; Wolverton, Chris; Dravid, Vinayak P.; Wu, Jinsong

doi:10.1038/s41467-019-09408-2

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

Journal Article · Fri Apr 12 00:00:00 EDT 2019 · Nature Communications

DOI:https://doi.org/10.1038/s41467-019-09408-2· OSTI ID:1510310

Li, Qianqian ^[1]; ^[2]; ^[3]; ^[4]; Thackeray, Michael M. ^[3]; Wolverton, Chris ^[4]; Dravid, Vinayak P. ^[4]; Wu, Jinsong ^[5]

Wuhan Univ. of Technology, Hubei (China); Shanghai Univ., Shanghai (China); Northwestern Univ., Evanston, IL (United States)
Northwestern Univ., Evanston, IL (United States); Harvard Univ., Cambridge, MA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Northwestern Univ., Evanston, IL (United States)
Wuhan Univ. of Technology, Hubei (China); Northwestern Univ., Evanston, IL (United States)

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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Electrical Energy Storage (CEES); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357

OSTI ID:: 1510310

Alternate ID(s):: OSTI ID: 1542887

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 10; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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