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

Cheng, Qian and Wei, Lu and Liu, Zhe and Ni, Nan and Sang, Zhe and Zhu, Bin and Xu, Weiheng and Chen, Meijie and Miao, Yupeng and Chen, Long-Qing and Min, Wei and Yang, Yuan (2018) Operando and three-dimensional visualization of anion depletion and lithium growth by stimulated Raman scattering microscopy. Nature Communications, 9 . Art. No. 2942. ISSN 2041-1723. PMCID PMC6065384.

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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.

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URLURL TypeDescription CentralArticle
Cheng, Qian0000-0001-5510-2977
Wei, Lu0000-0001-9170-2283
Zhu, Bin0000-0001-6165-3994
Min, Wei0000-0003-2570-3557
Yang, Yuan0000-0003-0264-2640
Additional Information:© 2018 The Author(s). Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit Received: 12 December 2017 Accepted: 24 June 2018. Published online: 30 July 2018. We acknowledge seed funding support from Columbia University’s Research Initiatives in Science & Engineering competition, started in 2004 to trigger high-risk, high-reward, and innovative collaborations in the basic sciences, engineering, and medicine. Y.Y. acknowledges support from startup funding by Columbia University. W.M. acknowledges support from the US Army Research Office (W911NF-12-1-0594), NIH Director’s New Innovator Award (1DP2EB016573) and R01 (EB020892), and the Camille and Henry Dreyfus Foundation. Z.L and L.-Q.C. acknowledge the support from the Department of Energy, Office of Energy Efficiency and Renewable Energy (EERE), under the Award (DE-EE0007803). Y.Y and Q.C. also want to thank Prof. Alan West at Columbia University for his kind help. These authors contributed equally: Qian Cheng, Lu Wei. Author Contributions: Y.Y., W.M., Q.C., and L.W. conceived the idea and designed the experiments. Q.C. and L.W. performed all the experiments and measurements. Z.L, Z.S. and L-Q. C. performed simulations. N.N., B.Z., W.X., M.C., and Y.M. helped prepare and perform experiments. All authors discussed the results. Q.C., L.W., Y.Y., W.M. and Z.L. wrote the paper with the input from all authors. Data availability: The data that support the findings of this study are available from the corresponding author upon reasonable request. The authors declare no competing interests.
Funding AgencyGrant Number
Columbia UniversityUNSPECIFIED
Army Research Office (ARO)W911NF-12-1-0594
NIHR01 EB020892
Camille and Henry Dreyfus FoundationUNSPECIFIED
Department of Energy (DOE)DE-EE0007803
PubMed Central ID:PMC6065384
Record Number:CaltechAUTHORS:20181119-102039470
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:91010
Deposited By: George Porter
Deposited On:19 Nov 2018 21:50
Last Modified:09 Mar 2020 13:19

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