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Title: Quantitative Relationships Between Pore Tortuosity, Pore Topology, and Solid Particle Morphology Using a Novel Discrete Particle Size Algorithm

Abstract

To sustain the continuous high-rate charge current required for fast charging of electric vehicle batteries, the ionic effective diffusion coefficient of the electrodes must be high enough to avoid the electrode being transport limited. Tortuosity factor and porosity are the two microstructure parameters that control this effective diffusion coefficient. While different methods exist to experimentally measure or calculate the tortuosity factor, no generic relationship between tortuosity and microstructure presently exists that is applicable across a large variety of electrode microstructures and porosities. Indeed, most relationships are microstructure specific. In this work, generic relationships are established using only geometrically defined metrics that can thus be used to design thick electrodes suitable for fast charging. To achieve this objective, an original, discrete particle-size algorithm is introduced and used to identify and segment particles across a set of 19 various electrode microstructures (nickel-manganese-cobalt [NMC] and graphite) obtained from X-ray computed tomography (CT) to quantify parameters such as porosity, particle elongation, sinuosity, and constriction, which influence the effective diffusion coefficient. Compared to the widely used watershed method, the new algorithm shows less over-segmentation. Particle size obtained with different numerical methods is also compared. Lastly, microstructure-tortuosity relationship and particle size and morphology analysis methods aremore » reviewed.« less

Authors:
ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; Faraday Institution
OSTI Identifier:
1631781
Alternate Identifier(s):
OSTI ID: 1660059; OSTI ID: 1660757
Report Number(s):
NREL/JA-5400-75813
Journal ID: ISSN 1945-7111
Grant/Contract Number:  
AC36-08GO28308; FIRG001; AC02-06CH11357
Resource Type:
Published Article
Journal Name:
Journal of the Electrochemical Society (Online)
Additional Journal Information:
Journal Name: Journal of the Electrochemical Society (Online) Journal Volume: 167 Journal Issue: 10; Journal ID: ISSN 1945-7111
Publisher:
IOP Publishing
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; electrode tortuosity factor; discrete particle size algorithm; particle identification; pore network; nickel-cobalt-manganese; graphite; Li-ion battery; Lithium-ion battery; fast charge

Citation Formats

Usseglio-Viretta, Francois L. E., Finegan, Donal P., Colclasure, Andrew, Heenan, Thomas M. M., Abraham, Daniel, Shearing, Paul, and Smith, Kandler. Quantitative Relationships Between Pore Tortuosity, Pore Topology, and Solid Particle Morphology Using a Novel Discrete Particle Size Algorithm. United States: N. p., 2020. Web. doi:10.1149/1945-7111/ab913b.
Usseglio-Viretta, Francois L. E., Finegan, Donal P., Colclasure, Andrew, Heenan, Thomas M. M., Abraham, Daniel, Shearing, Paul, & Smith, Kandler. Quantitative Relationships Between Pore Tortuosity, Pore Topology, and Solid Particle Morphology Using a Novel Discrete Particle Size Algorithm. United States. doi:https://doi.org/10.1149/1945-7111/ab913b
Usseglio-Viretta, Francois L. E., Finegan, Donal P., Colclasure, Andrew, Heenan, Thomas M. M., Abraham, Daniel, Shearing, Paul, and Smith, Kandler. Wed . "Quantitative Relationships Between Pore Tortuosity, Pore Topology, and Solid Particle Morphology Using a Novel Discrete Particle Size Algorithm". United States. doi:https://doi.org/10.1149/1945-7111/ab913b.
@article{osti_1631781,
title = {Quantitative Relationships Between Pore Tortuosity, Pore Topology, and Solid Particle Morphology Using a Novel Discrete Particle Size Algorithm},
author = {Usseglio-Viretta, Francois L. E. and Finegan, Donal P. and Colclasure, Andrew and Heenan, Thomas M. M. and Abraham, Daniel and Shearing, Paul and Smith, Kandler},
abstractNote = {To sustain the continuous high-rate charge current required for fast charging of electric vehicle batteries, the ionic effective diffusion coefficient of the electrodes must be high enough to avoid the electrode being transport limited. Tortuosity factor and porosity are the two microstructure parameters that control this effective diffusion coefficient. While different methods exist to experimentally measure or calculate the tortuosity factor, no generic relationship between tortuosity and microstructure presently exists that is applicable across a large variety of electrode microstructures and porosities. Indeed, most relationships are microstructure specific. In this work, generic relationships are established using only geometrically defined metrics that can thus be used to design thick electrodes suitable for fast charging. To achieve this objective, an original, discrete particle-size algorithm is introduced and used to identify and segment particles across a set of 19 various electrode microstructures (nickel-manganese-cobalt [NMC] and graphite) obtained from X-ray computed tomography (CT) to quantify parameters such as porosity, particle elongation, sinuosity, and constriction, which influence the effective diffusion coefficient. Compared to the widely used watershed method, the new algorithm shows less over-segmentation. Particle size obtained with different numerical methods is also compared. Lastly, microstructure-tortuosity relationship and particle size and morphology analysis methods are reviewed.},
doi = {10.1149/1945-7111/ab913b},
journal = {Journal of the Electrochemical Society (Online)},
number = 10,
volume = 167,
place = {United States},
year = {2020},
month = {6}
}

Journal Article:
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DOI: https://doi.org/10.1149/1945-7111/ab913b

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Works referenced in this record:

The Electrical Resistivity Log as an Aid in Determining Some Reservoir Characteristics
journal, December 1942

  • Archie, G. E.
  • Transactions of the AIME, Vol. 146, Issue 01
  • DOI: 10.2118/942054-G

A Simple Expression for the Tortuosity of Gas Transport Paths in Solid Oxide Fuel Cells’ Porous Electrodes
journal, December 2015


Mapping forces in a 3D elastic assembly of grains
journal, January 2012

  • Saadatfar, Mohammad; Sheppard, Adrian P.; Senden, Tim J.
  • Journal of the Mechanics and Physics of Solids, Vol. 60, Issue 1
  • DOI: 10.1016/j.jmps.2011.10.001

The use of mathematical modeling in the design of lithium/polymer battery systems
journal, October 1995


Quasi-Linear Algorithms for the Topological Watershed
journal, May 2005

  • Couprie, Michel; Najman, Laurent; Bertrand, Gilles
  • Journal of Mathematical Imaging and Vision, Vol. 22, Issue 2-3
  • DOI: 10.1007/s10851-005-4892-4

Anode microstructures from high-energy and high-power lithium-ion cylindrical cells obtained by X-ray nano-tomography
journal, December 2014


Analysis of diffusion in macroporous media in terms of a porosity, a tortuosity and a constrictivity factor
journal, September 1974


Topographic distance and watershed lines
journal, July 1994


Watershed Cuts: Minimum Spanning Forests and the Drop of Water Principle
journal, August 2009

  • Cousty, J.; Bertrand, G.; Najman, L.
  • IEEE Transactions on Pattern Analysis and Machine Intelligence, Vol. 31, Issue 8
  • DOI: 10.1109/TPAMI.2008.173

Gaseous diffusion in porous media. Part 2. - Dry granular materials
journal, August 1960


On tortuosity and the tortuosity factor in flow and diffusion through porous media
journal, January 1989


The influence of constrictivity on the effective transport properties of porous layers in electrolysis and fuel cells
journal, October 2012


Modeling of Particle-Particle Interactions in Porous Cathodes for Lithium-Ion Batteries
journal, January 2007

  • Stephenson, David E.; Hartman, Erik M.; Harb, John N.
  • Journal of The Electrochemical Society, Vol. 154, Issue 12
  • DOI: 10.1149/1.2783772

Quantitative Microstructure Characterization of a NMC Electrode
journal, July 2017

  • Usseglio-Viretta, François Laurent Emilien; Smith, Kandler
  • ECS Transactions, Vol. 77, Issue 11
  • DOI: 10.1149/07711.1095ecst

Nickel–Zirconia Anode Degradation and Triple Phase Boundary Quantification from Microstructural Analysis
journal, December 2009


Priority-flood: An optimal depression-filling and watershed-labeling algorithm for digital elevation models
journal, January 2014


A Survey: Image Segmentation Techniques [A Survey: Image Segmentation Techniques]
journal, January 2014


Power and thermal characterization of a lithium-ion battery pack for hybrid-electric vehicles
journal, September 2006


TauFactor: An open-source application for calculating tortuosity factors from tomographic data
journal, January 2016


Simplification and order reduction of lithium-ion battery model based on porous-electrode theory
journal, January 2012


Diffusion in a pore of irregular cross section—a simplified treatment
journal, June 1959


3D geometry and topology of pore pathways in Opalinus clay: Implications for mass transport
journal, April 2011


Tortuosity in Porous Media: A Critical Review
journal, January 2013

  • Ghanbarian, Behzad; Hunt, Allen G.; Ewing, Robert P.
  • Soil Science Society of America Journal, Vol. 77, Issue 5
  • DOI: 10.2136/sssaj2012.0435

Graph theory applications to continuity and ranking in geologic models
journal, March 1999


Average Grain Size in Polycrystalline Ceramics
journal, August 1969


Enabling fast charging – Infrastructure and economic considerations
journal, November 2017


Medial axis analysis of void structure in three-dimensional tomographic images of porous media
journal, April 1996

  • Lindquist, W. Brent; Lee, Sang-Moon; Coker, David A.
  • Journal of Geophysical Research: Solid Earth, Vol. 101, Issue B4
  • DOI: 10.1029/95JB03039

The use of contrast enhancement techniques in X-ray imaging of lithium–ion battery electrodes
journal, November 2016

  • Taiwo, Oluwadamilola O.; Finegan, Donal P.; Gelb, Jeff
  • Chemical Engineering Science, Vol. 154
  • DOI: 10.1016/j.ces.2016.04.023

Local Structural Characteristics of Pore Space in GDLs of PEM Fuel Cells Based on Geometric 3D Graphs
journal, January 2009

  • Thiedmann, Ralf; Hartnig, Christoph; Manke, Ingo
  • Journal of The Electrochemical Society, Vol. 156, Issue 11
  • DOI: 10.1149/1.3222737

Pore Size Distributions in Porous Glasses:  A Computer Simulation Study
journal, January 1999


Control oriented 1D electrochemical model of lithium ion battery
journal, September 2007


Porous-electrode theory with battery applications
journal, January 1975


Quantifying tortuosity in porous Li-ion battery materials
journal, March 2009


Electrochemical Modeling of Lithium-Ion Positive Electrodes during Hybrid Pulse Power Characterization Tests
journal, January 2008

  • Dees, Dennis; Gunen, Evren; Abraham, Daniel
  • Journal of The Electrochemical Society, Vol. 155, Issue 8
  • DOI: 10.1149/1.2939211

Watersheds in digital spaces: an efficient algorithm based on immersion simulations
journal, June 1991

  • Vincent, L.; Soille, P.
  • IEEE Transactions on Pattern Analysis and Machine Intelligence, Vol. 13, Issue 6
  • DOI: 10.1109/34.87344

On the origin and application of the Bruggeman correlation for analysing transport phenomena in electrochemical systems
journal, May 2016

  • Tjaden, Bernhard; Cooper, Samuel J.; Brett, Daniel JL
  • Current Opinion in Chemical Engineering, Vol. 12
  • DOI: 10.1016/j.coche.2016.02.006

Microstructure degradation of cermet anodes for solid oxide fuel cells: Quantification of nickel grain growth in dry and in humid atmospheres
journal, February 2011


Enabling fast charging – A battery technology gap assessment
journal, November 2017


Determination of the size of the representative volume element for random composites: statistical and numerical approach
journal, June 2003


Modeling of Galvanostatic Charge and Discharge of the Lithium/Polymer/Insertion Cell
journal, January 1993

  • Doyle, Marc
  • Journal of The Electrochemical Society, Vol. 140, Issue 6
  • DOI: 10.1149/1.2221597

A linear time algorithm for computing exact Euclidean distance transforms of binary images in arbitrary dimensions
journal, February 2003

  • Maurer, C. R.; Raghavan, V.
  • IEEE Transactions on Pattern Analysis and Machine Intelligence, Vol. 25, Issue 2
  • DOI: 10.1109/TPAMI.2003.1177156

Surface area overestimation within three-dimensional digital images and its consequence for skeletal dosimetry
journal, April 2002

  • Rajon, D. A.; Patton, P. W.; Shah, A. P.
  • Medical Physics, Vol. 29, Issue 5
  • DOI: 10.1118/1.1470207

X-Ray Tomography for Lithium Ion Battery Research: A Practical Guide
journal, July 2017


Requirements for Enabling Extreme Fast Charging of High Energy Density Li-Ion Cells while Avoiding Lithium Plating
journal, January 2019

  • Colclasure, Andrew M.; Dunlop, Alison R.; Trask, Stephen E.
  • Journal of The Electrochemical Society, Vol. 166, Issue 8
  • DOI: 10.1149/2.0451908jes

Hybrid image segmentation using watersheds and fast region merging
journal, January 1998

  • Haris, K.; Efstratiadis, S. N.; Maglaveras, N.
  • IEEE Transactions on Image Processing, Vol. 7, Issue 12
  • DOI: 10.1109/83.730380

Theoretical Analysis of Current Distribution in Porous Electrodes
journal, January 1962

  • Newman, John S.; Tobias, Charles W.
  • Journal of The Electrochemical Society, Vol. 109, Issue 12
  • DOI: 10.1149/1.2425269

Contradicting Geometrical Concepts in Pore Size Analysis Attained with Electron Microscopy and Mercury Intrusion
journal, December 2008


Tortuosity Anisotropy in Lithium-Ion Battery Electrodes
journal, October 2013

  • Ebner, Martin; Chung, Ding-Wen; García, R. Edwin
  • Advanced Energy Materials, Vol. 4, Issue 5
  • DOI: 10.1002/aenm.201301278

Enabling fast charging – Battery thermal considerations
journal, November 2017


Critical review of the impact of tortuosity on diffusion
journal, July 2007


The application of phase contrast X-ray techniques for imaging Li-ion battery electrodes
journal, April 2014

  • Eastwood, D. S.; Bradley, R. S.; Tariq, F.
  • Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 324
  • DOI: 10.1016/j.nimb.2013.08.066

Magnetically aligned graphite electrodes for high-rate performance Li-ion batteries
journal, July 2016

  • Billaud, Juliette; Bouville, Florian; Magrini, Tommaso
  • Nature Energy, Vol. 1, Issue 8
  • DOI: 10.1038/nenergy.2016.97

One parameter is always enough
journal, September 2018


Quantitative Characterization of LiFePO 4 Cathodes Reconstructed by FIB/SEM Tomography
journal, January 2012

  • Ender, Moses; Joos, Jochen; Carraro, Thomas
  • Journal of The Electrochemical Society, Vol. 159, Issue 7
  • DOI: 10.1149/2.033207jes

Multi-Domain Modeling of Lithium-Ion Batteries Encompassing Multi-Physics in Varied Length Scales
journal, January 2011

  • Kim, Gi-Heon; Smith, Kandler; Lee, Kyu-Jin
  • Journal of The Electrochemical Society, Vol. 158, Issue 8
  • DOI: 10.1149/1.3597614

FIB-Nanotomography of Particulate Systems—Part II: Particle Recognition and Effect of Boundary Truncation
journal, August 2006


Enabling fast charging – Vehicle considerations
journal, November 2017


Tortuosity in electrochemical devices: a review of calculation approaches
journal, November 2016


Review of simplified Pseudo-two-Dimensional models of lithium-ion batteries
journal, September 2016


Diffusion in a pore of varying cross section
journal, September 1958