Operando and three-dimensional visualization of anion depletion and lithium growth by stimulated Raman scattering microscopy

Qian Cheng, Lu Wei, Zhe Liu, Nan Ni, Zhe Sang, Bin Zhu, Weiheng Xu, Meijie Chen, Yupeng Miao, Long-Qing Chen, Wei Min () and Yuan Yang ()
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Qian Cheng: Program of Materials Science and Engineering, Columbia University
Lu Wei: Columbia University
Zhe Liu: The Pennsylvania State University
Nan Ni: Program of Materials Science and Engineering, Columbia University
Zhe Sang: Program of Materials Science and Engineering, Columbia University
Bin Zhu: Program of Materials Science and Engineering, Columbia University
Weiheng Xu: Program of Materials Science and Engineering, Columbia University
Meijie Chen: Program of Materials Science and Engineering, Columbia University
Yupeng Miao: Columbia University
Long-Qing Chen: The Pennsylvania State University
Wei Min: Columbia University
Yuan Yang: Program of Materials Science and Engineering, Columbia University

Nature Communications, 2018, vol. 9, issue 1, 1-10

Abstract: Abstract Visualization of ion transport in electrolytes provides fundamental understandings of electrolyte dynamics and electrolyte-electrode interactions. However, this is challenging because existing techniques are hard to capture low ionic concentrations and fast electrolyte dynamics. Here we show that stimulated Raman scattering microscopy offers required resolutions to address a long-lasting question: how does the lithium-ion concentration correlate to uneven lithium deposition? In this study, anions are used to represent lithium ions since their concentrations should not deviate for more than 0.1 mM, even near nanoelectrodes. A three-stage lithium deposition process is uncovered, corresponding to no depletion, partial depletion, and full depletion of lithium ions. Further analysis reveals a feedback mechanism between the lithium dendrite growth and heterogeneity of local ionic concentration, which can be suppressed by artificial solid electrolyte interphase. This study shows that stimulated Raman scattering microscopy is a powerful tool for the materials and energy field.

Date: 2018
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DOI: 10.1038/s41467-018-05289-z

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