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Direct Visualization of Solid Electrolyte Interphase Formation in Lithium-Ion Batteries with In Situ Electrochemical Transmission Electron Microscopy

Published online by Cambridge University Press:  04 July 2014

Raymond R. Unocic*
Oak Ridge National Laboratory, Center for Nanophase Materials Sciences, Oak Ridge, TN 37831, USA
Xiao-Guang Sun
Oak Ridge National Laboratory, Chemical Sciences Division, Oak Ridge, TN 37831, USA
Robert L. Sacci
Oak Ridge National Laboratory, Materials Science and Technology Division, Oak Ridge, TN 37831, USA
Leslie A. Adamczyk
Oak Ridge National Laboratory, Materials Science and Technology Division, Oak Ridge, TN 37831, USA
Daan Hein Alsem
Hummingbird Scientific, Lacey, WA 98516, USA
Sheng Dai
Oak Ridge National Laboratory, Chemical Sciences Division, Oak Ridge, TN 37831, USA
Nancy J. Dudney
Oak Ridge National Laboratory, Materials Science and Technology Division, Oak Ridge, TN 37831, USA
Karren L. More
Oak Ridge National Laboratory, Center for Nanophase Materials Sciences, Oak Ridge, TN 37831, USA
*Corresponding author.
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Complex, electrochemically driven transport processes form the basis of electrochemical energy storage devices. The direct imaging of electrochemical processes at high spatial resolution and within their native liquid electrolyte would significantly enhance our understanding of device functionality, but has remained elusive. In this work we use a recently developed liquid cell for in situ electrochemical transmission electron microscopy to obtain insight into the electrolyte decomposition mechanisms and kinetics in lithium-ion (Li-ion) batteries by characterizing the dynamics of solid electrolyte interphase (SEI) formation and evolution. Here we are able to visualize the detailed structure of the SEI that forms locally at the electrode/electrolyte interface during lithium intercalation into natural graphite from an organic Li-ion battery electrolyte. We quantify the SEI growth kinetics and observe the dynamic self-healing nature of the SEI with changes in cell potential.

FEMMS Special Issue
© Microscopy Society of America 2014 

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