Generalised single particle models for high-rate operation of graded lithium-ion electrodes: Systematic derivation and validation
Generalised single particle models for high-rate operation of graded lithium-ion electrodes: Systematic derivation and validation
A derivation of the single particle (SP) model is made from a Doyle-Fuller-Newman (DFN) model for electrodes composed of uniformly sized spherical electrode particles of one chemistry. The derivation uses a formal asymptotic method based on the disparity between the size of the thermal voltage and that of the characteristic change in overpotential that occurs during (de)lithiation. Comparison is made be- tween the SP model and the DFN model for electrodes made from: lithium nickel manganese cobalt oxide (NMC), graphite and lithium iron phosphate (LFP). These are used to identify regimes where the SP model is accurate. For most chemistries, even at moderate rates, there are discrepancies between the DFN model and the SP model due to spatial non-uniformities in the electrolyte. Motivated by these discrepancies a correction term to the SP model is derived. Incorporating this into the SP model gives the corrected SP (cSP) model whose accuracy is very significantly improved over the SP model. Generalised versions of the cSP model for graded electrodes containing multiple electrode particle sizes (or chem- istries) in different regions of the electrode, are also derived. The results of this generalisation to the cSP model compare favourably to the full DFN model, even at relatively high discharge rates, where the active electrode material is either graphite or a particular NMC variant.
Single Particle Model, Newman model,
Richardson, Giles
3fd8e08f-e615-42bb-a1ff-3346c5847b91
Korotkin, Ivan
1ca96363-075e-41d9-a0c1-153c8c0cc31a
Ranom, Rahifa
85a9672a-ea74-48db-8302-6d1f3dd8a68d
Castle, Michael
f712c296-85c1-41c4-a7e4-3f9beaa2bd15
Foster, Jamie
4a0f392a-793f-4b89-b602-9edc16aef507
10 April 2020
Richardson, Giles
3fd8e08f-e615-42bb-a1ff-3346c5847b91
Korotkin, Ivan
1ca96363-075e-41d9-a0c1-153c8c0cc31a
Ranom, Rahifa
85a9672a-ea74-48db-8302-6d1f3dd8a68d
Castle, Michael
f712c296-85c1-41c4-a7e4-3f9beaa2bd15
Foster, Jamie
4a0f392a-793f-4b89-b602-9edc16aef507
Richardson, Giles, Korotkin, Ivan, Ranom, Rahifa, Castle, Michael and Foster, Jamie
(2020)
Generalised single particle models for high-rate operation of graded lithium-ion electrodes: Systematic derivation and validation.
Electrochimica Acta, 339, [135862].
(doi:10.1016/j.electacta.2020.135862).
Abstract
A derivation of the single particle (SP) model is made from a Doyle-Fuller-Newman (DFN) model for electrodes composed of uniformly sized spherical electrode particles of one chemistry. The derivation uses a formal asymptotic method based on the disparity between the size of the thermal voltage and that of the characteristic change in overpotential that occurs during (de)lithiation. Comparison is made be- tween the SP model and the DFN model for electrodes made from: lithium nickel manganese cobalt oxide (NMC), graphite and lithium iron phosphate (LFP). These are used to identify regimes where the SP model is accurate. For most chemistries, even at moderate rates, there are discrepancies between the DFN model and the SP model due to spatial non-uniformities in the electrolyte. Motivated by these discrepancies a correction term to the SP model is derived. Incorporating this into the SP model gives the corrected SP (cSP) model whose accuracy is very significantly improved over the SP model. Generalised versions of the cSP model for graded electrodes containing multiple electrode particle sizes (or chem- istries) in different regions of the electrode, are also derived. The results of this generalisation to the cSP model compare favourably to the full DFN model, even at relatively high discharge rates, where the active electrode material is either graphite or a particular NMC variant.
Text
EPMs_EcAc_resub_v2
- Accepted Manuscript
More information
Accepted/In Press date: 5 February 2020
e-pub ahead of print date: 19 February 2020
Published date: 10 April 2020
Additional Information:
Funding Information:
GR, IK and JF were supported by the Faraday Institution Multi-Scale Modelling (MSM) project Grant number EP/S003053/1 . MC acknowledges funding from the University Alliance, Doctoral Training Alliance. The authors are very grateful for the help of Dr. Simon O'Kane in fitting data for the electrode and electrolyte properties.
Publisher Copyright:
© 2020 Elsevier Ltd
Keywords:
Single Particle Model, Newman model,
Identifiers
Local EPrints ID: 438821
URI: http://eprints.soton.ac.uk/id/eprint/438821
ISSN: 0013-4686
PURE UUID: 0fa38968-d5c6-40cf-8aca-7799a7d18d6e
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Date deposited: 25 Mar 2020 17:30
Last modified: 17 Mar 2024 05:25
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Author:
Rahifa Ranom
Author:
Michael Castle
Author:
Jamie Foster
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