Editors' Choice—Mesoscale Analysis of Conductive Binder Domain Morphology in Lithium-Ion Battery Electrodes

Trembacki, Bradley L.; Mistry, Aashutosh N.; Noble, David R.; Ferraro, Mark E.; Mukherjee, Partha P.; Roberts, Scott A.

doi:10.1149/2.0981813jes

Title: Editors' Choice—Mesoscale Analysis of Conductive Binder Domain Morphology in Lithium-Ion Battery Electrodes

Journal Article · Tue Oct 16 00:00:00 EDT 2018 · Journal of the Electrochemical Society

DOI:https://doi.org/10.1149/2.0981813jes· OSTI ID:1477810

;

; Noble, David R.; Ferraro, Mark E.; Mukherjee, Partha P.;

Typical lithium-ion battery electrodes are porous composites comprised of active material, conductive additives, and polymeric binder, with liquid electrolyte filling the pores. The mesoscale morphology of these constituent phases has a significant impact on both electrochemical reactions and transport across the electrode, which can ultimately limit macroscale battery performance. We reconstruct published X-ray computed tomography (XCT) data from a NMC333 cathode to study mesoscale electrode behavior on an as-manufactured electrode geometry. We present and compare two distinct models that computationally generate a composite binder domain (CBD) phase that represents both the polymeric binder and conductive additives. We compare the effect of the resulting CBD morphologies on electrochemically active area, pore phase tortuosity, and effective electrical conductivity. Both dense and nanoporous CBD are considered, and we observe that acknowledging CBD nanoporosity significantly increases effective electrical conductivity by up to an order of magnitude. Properties are compared to published measurements as well as to approximate values often used in homogenized battery-scale models. All reconstructions exhibit less than 20% of the standard electrochemically active area approximation. Order of magnitude discrepancies are observed between two popular transport simulation numerical schemes (finite element method and finite volume method), highlighting the importance of careful numerical verification.

View Journal Article

Cite

Export

Save

Research Organization:: Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)

Grant/Contract Number:: AC04-94AL85000; NA0003525

OSTI ID:: 1477810

Alternate ID(s):: OSTI ID: 1483974

Report Number(s):: SAND-2018-11856J; /jes/165/13/E725.atom

Journal Information:: Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Vol. 165 Journal Issue: 13; ISSN 0013-4651

Publisher:: The Electrochemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 82 works

Citation information provided by
Web of Science

References (59)

Theory of Impedance Response of Porous Electrodes: Simplifications, Inhomogeneities, Non-Stationarities and Applications Huang, Jun; Zhang, Jianbo Journal of The Electrochemical Society, Vol. 163, Issue 9 https://doi.org/10.1149/2.0901609jes	journal	January 2016
Optimization of Acetylene Black Conductive Additive and PVDF Composition for High-Power Rechargeable Lithium-Ion Cells Liu, G.; Zheng, H.; Simens, A. S. Journal of The Electrochemical Society, Vol. 154, Issue 12 https://doi.org/10.1149/1.2792293	journal	January 2007
Modeling 3D Microstructure and Ion Transport in Porous Li-Ion Battery Electrodes Stephenson, David E.; Walker, Bryce C.; Skelton, Cole B. Journal of The Electrochemical Society, Vol. 158, Issue 7 https://doi.org/10.1149/1.3579996	journal	January 2011
Analysis of Long-Range Interaction in Lithium-Ion Battery Electrodes Mistry, Aashutosh; Juarez-Robles, Daniel; Stein, Malcolm Journal of Electrochemical Energy Conversion and Storage, Vol. 13, Issue 3 https://doi.org/10.1115/1.4035198	journal	August 2016
Direct Measurements of Effective Electronic Transport in Porous Li-Ion Electrodes Peterson, Serena W.; Wheeler, Dean R. Journal of The Electrochemical Society, Vol. 161, Issue 14 https://doi.org/10.1149/2.0661414jes	journal	January 2014
Experiment and simulation of the fabrication process of lithium-ion battery cathodes for determining microstructure and mechanical properties Forouzan, Mehdi M.; Chao, Chien-Wei; Bustamante, Danilo Journal of Power Sources, Vol. 312 https://doi.org/10.1016/j.jpowsour.2016.02.014	journal	April 2016
Lithium Batteries and Cathode Materials Whittingham, M. Stanley Chemical Reviews, Vol. 104, Issue 10, p. 4271-4302 https://doi.org/10.1021/cr020731c	journal	October 2004
A Framework for Three-Dimensional Mesoscale Modeling of Anisotropic Swelling and Mechanical Deformation in Lithium-Ion Electrodes Roberts, Scott A.; Brunini, Victor E.; Long, Kevin N. Journal of The Electrochemical Society, Vol. 161, Issue 11 https://doi.org/10.1149/2.0081411jes	journal	January 2014
Transport-Geometry Interactions in Li-Ion Cathode Materials Imaged Using X-ray Nanotomography Nelson, George J.; Ausderau, Logan J.; Shin, SeungYoon Journal of The Electrochemical Society, Vol. 164, Issue 7 https://doi.org/10.1149/2.0261707jes	journal	January 2017
A comprehensive understanding of electrode thickness effects on the electrochemical performances of Li-ion battery cathodes Zheng, Honghe; Li, Jing; Song, Xiangyun Electrochimica Acta, Vol. 71, p. 258-265 https://doi.org/10.1016/j.electacta.2012.03.161	journal	June 2012
Three-Phase Multiscale Modeling of a LiCoO ₂ Cathode: Combining the Advantages of FIB-SEM Imaging and X-Ray Tomography Zielke, Lukas; Hutzenlaub, Tobias; Wheeler, Dean R. Advanced Energy Materials, Vol. 5, Issue 5 https://doi.org/10.1002/aenm.201401612	journal	November 2014
A conformal decomposition finite element method for modeling stationary fluid interface problems Noble, David R.; Newren, Elijah P.; Lechman, Jeremy B. International Journal for Numerical Methods in Fluids https://doi.org/10.1002/fld.2095	journal	January 2009
Materials Challenges and Opportunities of Lithium Ion Batteries Manthiram, Arumugam The Journal of Physical Chemistry Letters, Vol. 2, Issue 3 https://doi.org/10.1021/jz1015422	journal	January 2011
Lithiation-Induced Dilation Mapping in a Lithium-Ion Battery Electrode by 3D X-Ray Microscopy and Digital Volume Correlation Eastwood, David S.; Yufit, Vladimir; Gelb, Jeff Advanced Energy Materials, Vol. 4, Issue 4 https://doi.org/10.1002/aenm.201300506	journal	November 2013
Tortuosity of Battery Electrodes: Validation of Impedance-Derived Values and Critical Comparison with 3D Tomography Landesfeind, Johannes; Ebner, Martin; Eldiven, Askin Journal of The Electrochemical Society, Vol. 165, Issue 3 https://doi.org/10.1149/2.0231803jes	journal	January 2018
Three-dimensional high resolution X-ray imaging and quantification of lithium ion battery mesocarbon microbead anodes Tariq, F.; Yufit, V.; Kishimoto, M. Journal of Power Sources, Vol. 248 https://doi.org/10.1016/j.jpowsour.2013.08.147	journal	February 2014
X-Ray Tomography of Porous, Transition Metal Oxide Based Lithium Ion Battery Electrodes Ebner, Martin; Geldmacher, Felix; Marone, Federica Advanced Energy Materials, Vol. 3, Issue 7 https://doi.org/10.1002/aenm.201200932	journal	March 2013
FIB/SEM-based calculation of tortuosity in a porous LiCoO2 cathode for a Li-ion battery Hutzenlaub, T.; Asthana, A.; Becker, J. Electrochemistry Communications, Vol. 27 https://doi.org/10.1016/j.elecom.2012.11.006	journal	February 2013
Morphology of nanoporous carbon-binder domains in Li-ion batteries—A FIB-SEM study Vierrath, Severin; Zielke, Lukas; Moroni, Riko Electrochemistry Communications, Vol. 60 https://doi.org/10.1016/j.elecom.2015.09.010	journal	November 2015
4D analysis of the microstructural evolution of Si-based electrodes during lithiation: Time-lapse X-ray imaging and digital volume correlation Paz-Garcia, J. M.; Taiwo, O. O.; Tudisco, E. Journal of Power Sources, Vol. 320 https://doi.org/10.1016/j.jpowsour.2016.04.076	journal	July 2016
Local Tortuosity Inhomogeneities in a Lithium Battery Composite Electrode Kehrwald, Dirk; Shearing, Paul R.; Brandon, Nigel P. Journal of The Electrochemical Society, Vol. 158, Issue 12 https://doi.org/10.1149/2.079112jes	journal	January 2011
Critical electrode properties and drying conditions causing component segregation in graphitic anodes for lithium-ion batteries Westphal, Bastian G.; Kwade, Arno Journal of Energy Storage, Vol. 18 https://doi.org/10.1016/j.est.2018.06.009	journal	August 2018
Conductivity Degradation of Polyvinylidene Fluoride Composite Binder during Cycling: Measurements and Simulations for Lithium-Ion Batteries Grillet, Anne M.; Humplik, Thomas; Stirrup, Emily K. Journal of The Electrochemical Society, Vol. 163, Issue 9 https://doi.org/10.1149/2.0341609jes	journal	January 2016
A conformal decomposition finite element method for arbitrary discontinuities on moving interfaces: CDFEM FOR ARBITRARY DISCONTINUITIES ON MOVING INTERFACES Kramer, Richard M. J.; Noble, David R. International Journal for Numerical Methods in Engineering, Vol. 100, Issue 2 https://doi.org/10.1002/nme.4717	journal	June 2014
A review of conduction phenomena in Li-ion batteries Park, Myounggu; Zhang, Xiangchun; Chung, Myoungdo Journal of Power Sources, Vol. 195, Issue 24 https://doi.org/10.1016/j.jpowsour.2010.06.060	journal	December 2010
Insights Into Lithium-Ion Battery Degradation and Safety Mechanisms From Mesoscale Simulations Using Experimentally Reconstructed Mesostructures Roberts, Scott A.; Mendoza, Hector; Brunini, Victor E. Journal of Electrochemical Energy Conversion and Storage, Vol. 13, Issue 3 https://doi.org/10.1115/1.4034410	journal	August 2016
Batteries for Electric and Hybrid-Electric Vehicles Cairns, Elton J.; Albertus, Paul Annual Review of Chemical and Biomolecular Engineering, Vol. 1, Issue 1 https://doi.org/10.1146/annurev-chembioeng-073009-100942	journal	June 2010
Quantifying tortuosity in porous Li-ion battery materials Thorat, Indrajeet V.; Stephenson, David E.; Zacharias, Nathan A. Journal of Power Sources, Vol. 188, Issue 2 https://doi.org/10.1016/j.jpowsour.2008.12.032	journal	March 2009
A verified conformal decomposition finite element method for implicit, many-material geometries Roberts, Scott A.; Mendoza, Hector; Brunini, Victor E. Journal of Computational Physics, Vol. 375 https://doi.org/10.1016/j.jcp.2018.08.022	journal	December 2018
Cooperation between Active Material, Polymeric Binder and Conductive Carbon Additive in Lithium Ion Battery Cathode Zheng, Honghe; Yang, Ruizhi; Liu, Gao The Journal of Physical Chemistry C, Vol. 116, Issue 7 https://doi.org/10.1021/jp208428w	journal	February 2012
Mechanistic Understanding of the Role of Evaporation in Electrode Processing Stein, Malcolm; Mistry, Aashutosh; Mukherjee, Partha P. Journal of The Electrochemical Society, Vol. 164, Issue 7 https://doi.org/10.1149/2.1271707jes	journal	January 2017
Particles and Polymer Binder Interaction: A Controlling Factor in Lithium-Ion Electrode Performance Liu, G.; Zheng, H.; Song, X. Journal of The Electrochemical Society, Vol. 159, Issue 3 https://doi.org/10.1149/2.024203jes	journal	January 2012
Mesoscale Effective Property Simulations Incorporating Conductive Binder Trembacki, Bradley L.; Noble, David R.; Brunini, Victor E. Journal of The Electrochemical Society, Vol. 164, Issue 11 https://doi.org/10.1149/2.0601711jes	journal	January 2017
Three-dimensional electrochemical Li-ion battery modelling featuring a focused ion-beam/scanning electron microscopy based three-phase reconstruction of a LiCoO2 cathode Hutzenlaub, T.; Thiele, S.; Paust, N. Electrochimica Acta, Vol. 115 https://doi.org/10.1016/j.electacta.2013.10.103	journal	January 2014
Modeling of Galvanostatic Charge and Discharge of the Lithium/Polymer/Insertion Cell Doyle, Marc Journal of The Electrochemical Society, Vol. 140, Issue 6 https://doi.org/10.1149/1.2221597	journal	January 1993
Image based modelling of microstructural heterogeneity in LiFePO 4 electrodes for Li-ion batteries Cooper, S. J.; Eastwood, D. S.; Gelb, J. Journal of Power Sources, Vol. 247 https://doi.org/10.1016/j.jpowsour.2013.04.156	journal	February 2014
Tortuosity Determination of Battery Electrodes and Separators by Impedance Spectroscopy Landesfeind, Johannes; Hattendorff, Johannes; Ehrl, Andreas Journal of The Electrochemical Society, Vol. 163, Issue 7 https://doi.org/10.1149/2.1141607jes	journal	January 2016
Micro-Four-Line Probe to Measure Electronic Conductivity and Contact Resistance of Thin-Film Battery Electrodes Lanterman, Bryson J.; Riet, Adriaan A.; Gates, Nathaniel S. Journal of The Electrochemical Society, Vol. 162, Issue 10 https://doi.org/10.1149/2.0581510jes	journal	January 2015
Challenges in the development of advanced Li-ion batteries: a review Etacheri, Vinodkumar; Marom, Rotem; Elazari, Ran Energy & Environmental Science, Vol. 4, Issue 9 https://doi.org/10.1039/c1ee01598b	journal	January 2011
X-Ray Tomography for Lithium Ion Battery Research: A Practical Guide Pietsch, Patrick; Wood, Vanessa Annual Review of Materials Research, Vol. 47, Issue 1 https://doi.org/10.1146/annurev-matsci-070616-123957	journal	July 2017
Effects of Various Conductive Additive and Polymeric Binder Contents on the Performance of a Lithium-Ion Composite Cathode Liu, G.; Zheng, H.; Kim, S. Journal of The Electrochemical Society, Vol. 155, Issue 12 https://doi.org/10.1149/1.2976031	journal	January 2008
A Combination of X-Ray Tomography and Carbon Binder Modeling: Reconstructing the Three Phases of LiCoO ₂ Li-Ion Battery Cathodes Zielke, Lukas; Hutzenlaub, Tobias; Wheeler, Dean R. Advanced Energy Materials, Vol. 4, Issue 8 https://doi.org/10.1002/aenm.201301617	journal	January 2014
Comparison of three-dimensional analysis and stereological techniques for quantifying lithium-ion battery electrode microstructures: COMPARISON AND TECHNIQUES FOR QUANTIFYING LITHIUM-ION BATTERY Taiwo, Oluwadamilola O.; Finegan, Donal P.; Eastwood, David S. Journal of Microscopy, Vol. 263, Issue 3 https://doi.org/10.1111/jmi.12389	journal	March 2016
Building better batteries Armand, M.; Tarascon, J.-M. Nature, Vol. 451, Issue 7179, p. 652-657 https://doi.org/10.1038/451652a	journal	February 2008
Tortuosity Anisotropy in Lithium-Ion Battery Electrodes Ebner, Martin; Chung, Ding-Wen; García, R. Edwin Advanced Energy Materials, Vol. 4, Issue 5 https://doi.org/10.1002/aenm.201301278	journal	October 2013
Berechnung verschiedener physikalischer Konstanten von heterogenen Substanzen. I. Dielektrizitätskonstanten und Leitfähigkeiten der Mischkörper aus isotropen Substanzen Bruggeman, D. A. G. Annalen der Physik, Vol. 416, Issue 7 https://doi.org/10.1002/andp.19354160705	journal	January 1935
Overcharge Performance of 3,7-Bis(trifluoromethyl)- N -ethylphenothiazine at High Concentration in Lithium-Ion Batteries Kaur, Aman Preet; Elliott, Corrine F.; Ergun, Selin Journal of The Electrochemical Society, Vol. 163, Issue 2 https://doi.org/10.1149/2.0951514jes	journal	October 2015
Numerical Heat Transfer and Fluid Flow Patankar, Suhas V. https://doi.org/10.1201/9781482234213	book	October 2018
Visualizing the Carbon Binder Phase of Battery Electrodes in Three Dimensions Daemi, Sohrab R.; Tan, Chun; Volkenandt, Tobias ACS Applied Energy Materials, Vol. 1, Issue 8 https://doi.org/10.1021/acsaem.8b00501	journal	July 2018
Microstructure formation of lithium-ion battery electrodes during drying – An ex-situ study using cryogenic broad ion beam slope-cutting and scanning electron microscopy (Cryo-BIB-SEM) Jaiser, Stefan; Kumberg, Jana; Klaver, Jop Journal of Power Sources, Vol. 345 https://doi.org/10.1016/j.jpowsour.2017.01.117	journal	March 2017
Multi Length Scale Microstructural Investigations of a Commercially Available Li-Ion Battery Electrode Shearing, P. R.; Brandon, N. P.; Gelb, J. Journal of The Electrochemical Society, Vol. 159, Issue 7 https://doi.org/10.1149/2.053207jes	journal	January 2012
Quantitative Characterization of LiFePO ₄ Cathodes Reconstructed by FIB/SEM Tomography Ender, Moses; Joos, Jochen; Carraro, Thomas Journal of The Electrochemical Society, Vol. 159, Issue 7 https://doi.org/10.1149/2.033207jes	journal	January 2012
Mechanical and Electrochemical Response of a LiCoO2 Cathode using Reconstructed Microstructures Mendoza, Hector; Roberts, Scott A.; Brunini, Victor E. Electrochimica Acta, Vol. 190 https://doi.org/10.1016/j.electacta.2015.12.224	journal	February 2016
Ionic Conduction in Lithium Ion Battery Composite Electrode Governs Cross-sectional Reaction Distribution Orikasa, Yuki; Gogyo, Yuma; Yamashige, Hisao Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/srep26382	journal	May 2016
Secondary-Phase Stochastics in Lithium-Ion Battery Electrodes Mistry, Aashutosh N.; Smith, Kandler; Mukherjee, Partha P. ACS Applied Materials & Interfaces, Vol. 10, Issue 7 https://doi.org/10.1021/acsami.7b17771	journal	January 2018
Analysis of geometric and electrochemical characteristics of lithium cobalt oxide electrode with different packing densities Lim, Cheolwoong; Yan, Bo; Kang, Huixiao Journal of Power Sources, Vol. 328 https://doi.org/10.1016/j.jpowsour.2016.07.119	journal	October 2016
Current distributions for a two-phase material with chequer-board geometry Soderberg, M.; Grimvall, G. Journal of Physics C: Solid State Physics, Vol. 16, Issue 6 https://doi.org/10.1088/0022-3719/16/6/014	journal	February 1983
Tool for Tortuosity Estimation in Lithium Ion Battery Porous Electrodes Ebner, Martin; Wood, Vanessa Journal of The Electrochemical Society, Vol. 162, Issue 2 https://doi.org/10.1149/2.0111502jes	journal	December 2014
Quantifying Bulk Electrode Strain and Material Displacement within Lithium Batteries via High-Speed Operando Tomography and Digital Volume Correlation Finegan, Donal P.; Tudisco, Erika; Scheel, Mario Advanced Science, Vol. 3, Issue 3 https://doi.org/10.1002/advs.201500332	journal	December 2015

Similar Records

Mesoscale Effects of Composition and Calendering in Lithium-Ion Battery Composite Electrodes

Journal Article · Tue Mar 10 00:00:00 EDT 2020 · Journal of Electrochemical Energy Conversion and Storage · OSTI ID:1477810

Trembacki, Bradley L.; Noble, David R.; Ferraro, Mark E.; +1 more

Mesoscale Effective Property Simulations Incorporating Conductive Binder

Journal Article · Wed Jul 26 00:00:00 EDT 2017 · Journal of the Electrochemical Society · OSTI ID:1477810

Trembacki, Bradley L.; Noble, David R.; Brunini, Victor E.; +2 more

Resolving the Discrepancy in Tortuosity Factor Estimation for Li-Ion Battery Electrodes through Micro-Macro Modeling and Experiment

Journal Article · Mon Jan 01 00:00:00 EST 2018 · Journal of the Electrochemical Society · OSTI ID:1477810

Usseglio-Viretta, Francois L. E.; Colclasure, Andrew; Mistry, Aashutosh N.; +10 more

Related Subjects

36 MATERIALS SCIENCE
25 ENERGY STORAGE
Batteries
Electrode Kinetics
Mesoscale
Tortuosity
Transport

Title: Editors' Choice—Mesoscale Analysis of Conductive Binder Domain Morphology in Lithium-Ion Battery Electrodes

Citation Formats

References (59)

Similar Records

Related Subjects