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

Journal Article · · Journal of the Electrochemical Society (Online)

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.

Research Organization:
National Renewable Energy Laboratory (NREL), Golden, CO (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; Faraday Institution; USDOE
Grant/Contract Number:
AC36-08GO28308; FIRG001; AC02-06CH11357
OSTI ID:
1631781
Alternate ID(s):
OSTI ID: 1660059; OSTI ID: 1660757
Report Number(s):
NREL/JA-5400-75813; MainId:6693; UUID:9fffce88-fd33-ea11-9c2f-ac162d87dfe5; MainAdminID:13843
Journal Information:
Journal of the Electrochemical Society (Online), Vol. 167, Issue 10; ISSN 1945-7111
Publisher:
IOP PublishingCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 32 works
Citation information provided by
Web of Science

References (72)

Review of simplified Pseudo-two-Dimensional models of lithium-ion batteries journal September 2016
Power and thermal characterization of a lithium-ion battery pack for hybrid-electric vehicles journal September 2006
Control oriented 1D electrochemical model of lithium ion battery journal September 2007
Multi-Domain Modeling of Lithium-Ion Batteries Encompassing Multi-Physics in Varied Length Scales journal January 2011
Efficient and Extensible Quasi-Explicit Modular Nonlinear Multiscale Battery Model: GH-MSMD journal January 2017
Simplification and order reduction of lithium-ion battery model based on porous-electrode theory journal January 2012
Modeling of Particle-Particle Interactions in Porous Cathodes for Lithium-Ion Batteries journal January 2007
Electrochemical Modeling of Lithium-Ion Positive Electrodes during Hybrid Pulse Power Characterization Tests journal January 2008
Comparing Macroscale and Microscale Simulations of Porous Battery Electrodes journal January 2017
Theoretical Analysis of Current Distribution in Porous Electrodes journal January 1962
Porous-electrode theory with battery applications journal January 1975
Modeling of Galvanostatic Charge and Discharge of the Lithium/Polymer/Insertion Cell journal January 1993
The use of mathematical modeling in the design of lithium/polymer battery systems journal October 1995
Resolving the Discrepancy in Tortuosity Factor Estimation for Li-Ion Battery Electrodes through Micro-Macro Modeling and Experiment journal January 2018
Requirements for Enabling Extreme Fast Charging of High Energy Density Li-Ion Cells while Avoiding Lithium Plating journal January 2019
Enabling fast charging – A battery technology gap assessment journal November 2017
Enabling fast charging – Battery thermal considerations journal November 2017
Enabling fast charging – Infrastructure and economic considerations journal November 2017
Enabling fast charging – Vehicle considerations journal November 2017
On tortuosity and the tortuosity factor in flow and diffusion through porous media journal January 1989
Tortuosity Determination of Battery Electrodes and Separators by Impedance Spectroscopy journal January 2016
TauFactor: An open-source application for calculating tortuosity factors from tomographic data journal January 2016
Characterisation of Solid Oxide Fuel Cell Ni–8YSZ substrate by synchrotron X-ray nano-tomography: from 3D reconstruction to microstructure quantification journal January 2012
Tortuosity in electrochemical devices: a review of calculation approaches journal November 2016
X-Ray Tomography for Lithium Ion Battery Research: A Practical Guide journal July 2017
The use of contrast enhancement techniques in X-ray imaging of lithium–ion battery electrodes journal November 2016
The application of phase contrast X-ray techniques for imaging Li-ion battery electrodes journal April 2014
Berechnung verschiedener physikalischer Konstanten von heterogenen Substanzen. I. Dielektrizitätskonstanten und Leitfähigkeiten der Mischkörper aus isotropen Substanzen journal January 1935
On the origin and application of the Bruggeman correlation for analysing transport phenomena in electrochemical systems journal May 2016
The Electrical Resistivity Log as an Aid in Determining Some Reservoir Characteristics journal December 1942
Quantifying tortuosity in porous Li-ion battery materials journal March 2009
Validity of the Bruggeman relation for porous electrodes journal October 2013
A Simple Expression for the Tortuosity of Gas Transport Paths in Solid Oxide Fuel Cells’ Porous Electrodes journal December 2015
Tortuosity in Porous Media: A Critical Review journal January 2013
Critical review of the impact of tortuosity on diffusion journal July 2007
Diffusion in a pore of varying cross section journal September 1958
Diffusion in a pore of irregular cross section—a simplified treatment journal June 1959
The influence of constrictivity on the effective transport properties of porous layers in electrolysis and fuel cells journal October 2012
Redox cycling of Ni–YSZ anodes for solid oxide fuel cells: Influence of tortuosity, constriction and percolation factors on the effective transport properties journal November 2013
Analysis of diffusion in macroporous media in terms of a porosity, a tortuosity and a constrictivity factor journal September 1974
Gaseous diffusion in porous media. Part 2. - Dry granular materials journal August 1960
Local Structural Characteristics of Pore Space in GDLs of PEM Fuel Cells Based on Geometric 3D Graphs journal January 2009
3D geometry and topology of pore pathways in Opalinus clay: Implications for mass transport journal April 2011
Medial axis analysis of void structure in three-dimensional tomographic images of porous media journal April 1996
Graph theory applications to continuity and ranking in geologic models journal March 1999
Microstructure degradation of cermet anodes for solid oxide fuel cells: Quantification of nickel grain growth in dry and in humid atmospheres journal February 2011
Quantitative Microstructure Characterization of a NMC Electrode journal July 2017
Tortuosity Anisotropy in Lithium-Ion Battery Electrodes journal October 2013
Magnetically aligned graphite electrodes for high-rate performance Li-ion batteries journal July 2016
Contradicting Geometrical Concepts in Pore Size Analysis Attained with Electron Microscopy and Mercury Intrusion journal December 2008
Pore Size Distributions in Porous Glasses:  A Computer Simulation Study journal January 1999
Determination of the size of the representative volume element for random composites: statistical and numerical approach journal June 2003
Off-lattice reconstruction of porous media: critical evaluation, geometrical confinement and molecular transport journal July 1998
Nickel–Zirconia Anode Degradation and Triple Phase Boundary Quantification from Microstructural Analysis journal December 2009
Average Grain Size in Polycrystalline Ceramics journal August 1969
Watersheds in digital spaces: an efficient algorithm based on immersion simulations journal June 1991
Topographic distance and watershed lines journal July 1994
Hybrid image segmentation using watersheds and fast region merging journal January 1998
Quasi-Linear Algorithms for the Topological Watershed journal May 2005
FIB-Nanotomography of Particulate Systems—Part II: Particle Recognition and Effect of Boundary Truncation journal August 2006
Watershed Cuts: Minimum Spanning Forests and the Drop of Water Principle journal August 2009
Mapping forces in a 3D elastic assembly of grains journal January 2012
Parallel Priority-Flood depression filling for trillion cell digital elevation models on desktops or clusters journal November 2016
A linear time algorithm for computing exact Euclidean distance transforms of binary images in arbitrary dimensions journal February 2003
Quantitative Characterization of LiFePO 4 Cathodes Reconstructed by FIB/SEM Tomography journal January 2012
Anode microstructures from high-energy and high-power lithium-ion cylindrical cells obtained by X-ray nano-tomography journal December 2014
Priority-flood: An optimal depression-filling and watershed-labeling algorithm for digital elevation models journal January 2014
Quantitative relationships between composition, particle size, triple phase boundary length and surface area in nickel-cermet anodes for Solid Oxide Fuel Cells journal September 2011
A Survey: Image Segmentation Techniques [A Survey: Image Segmentation Techniques] journal January 2014
Surface area overestimation within three-dimensional digital images and its consequence for skeletal dosimetry journal April 2002
The fractal nature of the three-phase boundary: A heuristic approach to the degradation of nanostructured solid oxide fuel cell anodes journal August 2017
One parameter is always enough journal September 2018