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Correlating Microstructural Lithium Metal Growth with Electrolyte Salt Depletion in Lithium Batteries Using 7Li MRI

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Department of Chemistry, Stony Brook University, Stony Brook, New York 11794-3400, United States
Department of Chemistry, New York University, 100 Washington Square East, New York, New York 10003, United States
§ Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, U.K.
Cite this: J. Am. Chem. Soc. 2015, 137, 48, 15209–15216
Publication Date (Web):November 2, 2015
Copyright © 2015 American Chemical Society

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    Lithium dendrite growth in lithium ion and lithium rechargeable batteries is associated with severe safety concerns. To overcome these problems, a fundamental understanding of the growth mechanism of dendrites under working conditions is needed. In this work, in situ 7Li magnetic resonance (MRI) is performed on both the electrolyte and lithium metal electrodes in symmetric lithium cells, allowing the behavior of the electrolyte concentration gradient to be studied and correlated with the type and rate of microstructure growth on the Li metal electrode. For this purpose, chemical shift (CS) imaging of the metal electrodes is a particularly sensitive diagnostic method, enabling a clear distinction to be made between different types of microstructural growth occurring at the electrode surface and the eventual dendrite growth between the electrodes. The CS imaging shows that mossy types of microstructure grow close to the surface of the anode from the beginning of charge in every cell studied, while dendritic growth is triggered much later. Simple metrics have been developed to interpret the MRI data sets and to compare results from a series of cells charged at different current densities. The results show that at high charge rates, there is a strong correlation between the onset time of dendrite growth and the local depletion of the electrolyte at the surface of the electrode observed both experimentally and predicted theoretical (via the Sand’s time model). A separate mechanism of dendrite growth is observed at low currents, which is not governed by salt depletion in the bulk liquid electrolyte. The MRI approach presented here allows the rate and nature of a process that occurs in the solid electrode to be correlated with the concentrations of components in the electrolyte.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/jacs.5b09385.

    • Pulse sequences, results for the cells charged at 0.16 and 1.26 mA cm–2, descriptions and examples of the CSI deconvolution and quantification of the electrolyte depletion, and the electrochemistry for all of the cells studied (PDF)

    • Movie showing MRI images acquired as a function of time for the cell charged at 0.16 mA cm–2 (MOV)

    • Movie showing MRI images acquired as a function of time for the cell charged at 0.32 mA cm–2 (MOV)

    • Movie showing MRI images acquired as a function of time for the cell charged at 0.51 mA cm–2 (MOV)

    • Movie showing MRI images acquired as a function of time for the cell charged at 0.76 mA cm–2 (MOV)

    • Movie showing MRI images acquired as a function of time for the cell charged at 1.01 mA cm–2 (MOV)

    • Movie showing MRI images acquired as a function of time for the cell charged at 1.26 mA cm–2 (MOV)

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