Abstract
In high energy density lithium metal batteries (LMBs), dendrite and solid electrolyte interphase (SEI) growth reduce safety and longevity, respectively. A stable SEI layer enables high efficiency cycling but continued SEI growth can lead to reduced capacity and coulombic efficiency. In this paper, we develop a steady-state model that predicts the effect of small advective electrolyte flow towards the lithium metal electrode on SEI growth during charging. For a fixed current density, increasing the electrolyte flow rate improves the coulombic efficiency and decreases SEI layer growth rate. Decreasing the charging current density at a constant flow rate also decreases the SEI layer growth rate. Low flow rates (μm/s) can increase coulombic efficiency by up to 6%. The sensitivity of the coulombic efficiency to plating and SEI layer reaction rates is also explored.
Highlights
Lithium metal batteries are promising, energy-dense generation batteries (Whittingham, 2012)
This paper develops the first steady-state model of a lithium metal electrode with normal electrolyte flow that includes solvent diffusion and solid electrolyte interphase (SEI) layer growth kinetics
Our previous analysis (Parekh et al, 2020) shows that at steady state, critical flow rate or Pe = Pecr leads to an almost uniform concentration profile given by c = 1 and we use that to calculate Pecr
Summary
Lithium metal batteries are promising, energy-dense generation batteries (Whittingham, 2012). Pinson and Bazant (2012) derive the square root dependence of long term SEI layer growth on time using single particle and porous electrode models and a solvent diffusion limited growth mechanism. Their models fit the experimental data obtained by Broussely et al (2001), Smith et al (2011). This paper develops the first steady-state model of a lithium metal electrode with normal electrolyte flow that includes solvent diffusion and SEI layer growth kinetics. To the best of authors’ knowledge, there has been no previous experimental study on the effect of electrolyte flow on SEI growth and the authors intend to explore that in the future
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