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Incorporating dendrite growth into continuum models of electrolytes: Insights from NMR measurements and inverse modeling

Incorporating dendrite growth into continuum models of electrolytes: Insights from NMR measurements and inverse modeling
Incorporating dendrite growth into continuum models of electrolytes: Insights from NMR measurements and inverse modeling
In this work we develop a combined experimental and inverse continuum modeling approach to the problem of determining properties of a lithium electrolyte from NMR measurements of ion concentration in a test cell. The experimental set-up consists of an enclosed, lithium-electrolyte-filled tube with lithium electrodes at either end. A constant current is passed between these electrodes and the resulting evolution of the spatial distribution of the lithium ions is monitored using NMR imaging techniques. Using the recently developed tools of inverse modeling, in combination with the concentration measurements acquired with NMR imaging, it is shown that the standard Planck-Nernst electrolyte model results in predictions of negative transference numbers. The observation of growing lithium dendrites on the cathode suggests the cause for these unphysical predictions and motivates the formulation of a generalized Planck-Nernst model that explicitly accounts for the presence of these growing lithium-metal dendrites. In this approach, lithium depletion in a dendritic region adjacent to the cathode is modelled by adding a suitably-chosen spatially distributed sink term. It is demonstrated that a model in which lithium is lost from the electrolyte uniformly throughout the dendritic region provides predictions of electrolyte data consistent with the literature and thereby remedies the shortcoming of the standard Planck-Nernst model. In addition, a state-of-the-art Bayesian technique is used to quantify the uncertainty of the inferred material properties.
0013-4651
A1591-A1602
Sethurajan, Athinthra
59e4e97e-c240-4793-8bb5-f26a853e3e5a
Foster, Jamie
a58f610d-d0e9-460f-9faa-35722fe75fcd
Richardson, Giles
3fd8e08f-e615-42bb-a1ff-3346c5847b91
Krachivovsky, Sergey
d84f9afe-ed5d-4a73-b409-f734e614c0d4
Bazak, David
743ef15d-26eb-467f-8216-7544edc9269c
Goward, Gillian
5e1924d6-8443-4a7f-a2aa-ffa3fbde7caa
Protas, Bartosz
49c1fe89-1cfc-414e-a961-6a75c25b946b
Sethurajan, Athinthra
59e4e97e-c240-4793-8bb5-f26a853e3e5a
Foster, Jamie
a58f610d-d0e9-460f-9faa-35722fe75fcd
Richardson, Giles
3fd8e08f-e615-42bb-a1ff-3346c5847b91
Krachivovsky, Sergey
d84f9afe-ed5d-4a73-b409-f734e614c0d4
Bazak, David
743ef15d-26eb-467f-8216-7544edc9269c
Goward, Gillian
5e1924d6-8443-4a7f-a2aa-ffa3fbde7caa
Protas, Bartosz
49c1fe89-1cfc-414e-a961-6a75c25b946b

Sethurajan, Athinthra, Foster, Jamie, Richardson, Giles, Krachivovsky, Sergey, Bazak, David, Goward, Gillian and Protas, Bartosz (2019) Incorporating dendrite growth into continuum models of electrolytes: Insights from NMR measurements and inverse modeling. Journal of the Electrochemical Society, 166 (8), A1591-A1602. (doi:10.1149/2.0921908jes).

Record type: Article

Abstract

In this work we develop a combined experimental and inverse continuum modeling approach to the problem of determining properties of a lithium electrolyte from NMR measurements of ion concentration in a test cell. The experimental set-up consists of an enclosed, lithium-electrolyte-filled tube with lithium electrodes at either end. A constant current is passed between these electrodes and the resulting evolution of the spatial distribution of the lithium ions is monitored using NMR imaging techniques. Using the recently developed tools of inverse modeling, in combination with the concentration measurements acquired with NMR imaging, it is shown that the standard Planck-Nernst electrolyte model results in predictions of negative transference numbers. The observation of growing lithium dendrites on the cathode suggests the cause for these unphysical predictions and motivates the formulation of a generalized Planck-Nernst model that explicitly accounts for the presence of these growing lithium-metal dendrites. In this approach, lithium depletion in a dendritic region adjacent to the cathode is modelled by adding a suitably-chosen spatially distributed sink term. It is demonstrated that a model in which lithium is lost from the electrolyte uniformly throughout the dendritic region provides predictions of electrolyte data consistent with the literature and thereby remedies the shortcoming of the standard Planck-Nernst model. In addition, a state-of-the-art Bayesian technique is used to quantify the uncertainty of the inferred material properties.

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Accepted/In Press date: 29 March 2019
e-pub ahead of print date: 13 May 2019

Identifiers

Local EPrints ID: 431932
URI: http://eprints.soton.ac.uk/id/eprint/431932
ISSN: 0013-4651
PURE UUID: 884f8640-b413-406b-a3ba-4fa3eedefbb4

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Date deposited: 21 Jun 2019 16:30
Last modified: 04 Nov 2019 17:34

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