Visualizing non-equilibrium lithiation of spinel oxide via in situ transmission electron microscopy

Kai He, Sen Zhang, Jing Li, Xiqian Yu, Qingping Meng, Yizhou Zhu, Enyuan Hu, Ke Sun, Hongseok Yun, Xiao-Qing Yang, Yimei Zhu, Hong Gan, Yifei Mo, Eric A. Stach, Christopher B. Murray () and Dong Su ()
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Kai He: Brookhaven National Laboratory
Sen Zhang: University of Pennsylvania
Jing Li: Brookhaven National Laboratory
Xiqian Yu: Brookhaven National Laboratory
Qingping Meng: Brookhaven National Laboratory
Yizhou Zhu: University of Maryland
Enyuan Hu: Brookhaven National Laboratory
Ke Sun: Brookhaven National Laboratory
Hongseok Yun: University of Pennsylvania
Xiao-Qing Yang: Brookhaven National Laboratory
Yimei Zhu: Brookhaven National Laboratory
Hong Gan: Brookhaven National Laboratory
Yifei Mo: University of Maryland
Eric A. Stach: Brookhaven National Laboratory
Christopher B. Murray: University of Pennsylvania
Dong Su: Brookhaven National Laboratory

Nature Communications, 2016, vol. 7, issue 1, 1-9

Abstract: Abstract Spinel transition metal oxides are important electrode materials for lithium-ion batteries, whose lithiation undergoes a two-step reaction, whereby intercalation and conversion occur in a sequential manner. These two reactions are known to have distinct reaction dynamics, but it is unclear how their kinetics affects the overall electrochemical response. Here we explore the lithiation of nanosized magnetite by employing a strain-sensitive, bright-field scanning transmission electron microscopy approach. This method allows direct, real-time, high-resolution visualization of how lithiation proceeds along specific reaction pathways. We find that the initial intercalation process follows a two-phase reaction sequence, whereas further lithiation leads to the coexistence of three distinct phases within single nanoparticles, which has not been previously reported to the best of our knowledge. We use phase-field theory to model and describe these non-equilibrium reaction pathways, and to directly correlate the observed phase evolution with the battery’s discharge performance.

Date: 2016
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DOI: 10.1038/ncomms11441

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