Separator-free and concentrated LiNO3 electrolyte cells enable uniform lithium electrodeposition

Rodrigo Rodriguez; Ruth A. Edison; Ryan M. Stephens; Ho-Hyun Sun; Adam Heller; C. Buddie Mullins

doi:10.1039/C9TA10929C

Separator-free and concentrated LiNO₃ electrolyte cells enable uniform lithium electrodeposition†

Rodrigo Rodriguez,^a Ruth A. Edison,^b Ryan M. Stephens,^f Ho-Hyun Sun,^a Adam Heller^ae and C. Buddie Mullins

*^acde

Author affiliations

* Corresponding authors

^a McKetta Department of Chemical Engineering, The University of Texas at Austin, Austin, Texas 78712-1589, USA
E-mail: mullins@che.utexas.edu

^b Department of Physics, The University of Texas at Austin, Austin, Texas 78712-1192, USA

^c Texas Materials Institute, The University of Texas at Austin, Austin, Texas 78712-1591, USA

^d Department of Chemistry, The University of Texas at Austin, Austin, Texas 78712-1224, USA

^e Center for Electrochemistry, The University of Texas at Austin, Austin, Texas 78712-0165, USA

^f Shell International Exploration & Production Inc., Houston, Texas 77082, USA

Abstract

Imaging of lithium electrodepositions revealed that in the absence of a compressed porous separator, achieved via a plastic washer, dendrite-free lithium was deposited from glyme solutions of 1 M LiNO₃. When the 1 M LiNO₃ in glyme was coupled with a 1 M LiFSI salt, high coulombic efficiencies were also attainable in both Li|Cu and anode-free LFP|Cu cells. However, dendrite resurgence was observed in cycled lithium coin cell electrodes when a porous separator was utilized. This was attributed to the restriction of Li⁺ flux to the electrode surface induced by the porous and tortuous structure of the polymer separator. At these pores, localized current densities, which exceeded the applied current density, and a non-uniform Li⁺ flux resulted in dendritic lithium growth. Replacement of the separator by a washer normalized the current distribution and provided for non-dendritic lithium deposits in coin cells.

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Article information

DOI: https://doi.org/10.1039/C9TA10929C
Article type: Paper
Submitted: 03 Oct 2019
Accepted: 27 Jan 2020
First published: 28 Jan 2020

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J. Mater. Chem. A, 2020,8, 3999-4006

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Separator-free and concentrated LiNO₃ electrolyte cells enable uniform lithium electrodeposition

R. Rodriguez, R. A. Edison, R. M. Stephens, H. Sun, A. Heller and C. B. Mullins, J. Mater. Chem. A, 2020, 8, 3999 DOI: 10.1039/C9TA10929C

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Journal of Materials Chemistry A