Abstract
Author(s): Frenck, L; Sethi, GK; Maslyn, JA; Balsara, NP | Abstract: Lithium metal is a promising anode material for next-generation rechargeable batteries, but non-uniform electrodeposition of lithium is a significant barrier. These non-uniform deposits are often referred to as lithium “dendrites,” although their morphologies can vary. We have surveyed the literature on lithium electrodeposition through three classes of electrolytes: liquids, polymers and inorganic solids. We find that the non-uniform deposits can be grouped into six classes: whiskers, moss, dendrites, globules, trees, and cracks. These deposits were obtained in a variety of cell geometries using both unidirectional deposition and cell cycling. The main result of the study is a figure where the morphology of electrodeposited lithium is plotted as a function of two variables: shear modulus of the electrolyte and current density normalized by the limiting current density. We show that specific morphologies are confined to contiguous regions on this two-dimensional plot.
Highlights
There is growing interest in the nature of electrodeposition at lithium metal electrodes due to the current focus on increasing the energy density of rechargeable lithium batteries (Girishkumar et al, 2010; Balsara and Newman, 2013)
While we have focused on the anode and the electrolyte, it is well-known that spontaneous reactions between lithium metal and all known electrolytes result in the formation of an solid electrolyte interphase (SEI) layer (Peled, 1979), which plays a central role in stable cycling (Tarascon and Armand, 2001; Meyerson et al, 2019)
We demonstrate that the lithium protrusion morphology obtained in different classes of electrolytes are mainly functions of two parameters: (1) current density normalized by the limiting current density and (2) modulus of the electrolyte
Summary
There is growing interest in the nature of electrodeposition at lithium metal electrodes due to the current focus on increasing the energy density of rechargeable lithium batteries (Girishkumar et al, 2010; Balsara and Newman, 2013). One of the main challenges is the nucleation and growth of protrusions during battery charging (Selim and Bro, 1974; Besenhard and Eichinger, 1976; Epelboin, 2006), which limits the battery lifetime and compromises safety (Yamaki et al, 1998; Aurbach et al, 2002). These protrusions are often referred to as “lithium dendrites.”. The passage of current results in salt concentration gradients in liquid-and polymer-based electrolytes (Chazalviel, 1990).
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