Quantifying Negative Effects of Carbon-Binder Networks from Electrochemical Performance of Porous Li-Ion Electrodes

Mistry, Aashutosh; Trask, Stephen; Dunlop, Alison; Jeka, Gerald; Polzin, Bryant; Mukherjee, Partha P.; Srinivasan, Venkat

doi:10.1149/1945-7111/ac1033

Title: Quantifying Negative Effects of Carbon-Binder Networks from Electrochemical Performance of Porous Li-Ion Electrodes

Journal Article · 20 July 2021 · Journal of the Electrochemical Society

DOI: https://doi.org/10.1149/1945-7111/ac1033 · OSTI ID:1831722

^[1];

^[2]; Dunlop, Alison ^[2]; Jeka, Gerald ^[2]; Polzin, Bryant ^[2];

^[3];

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Argonne National Lab. (ANL), Lemont, IL (United States); Purdue Univ., West Lafayette, IN (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)
Purdue Univ., West Lafayette, IN (United States)
Argonne National Lab. (ANL), Lemont, IL (United States). Joint Center for Energy Storage Research (JCESR); Argonne National Lab. (ANL), Lemont, IL (United States). Argonne Collaborative Center for Energy Storage Science

Porous Li-ion electrodes contain active particles, ion transporting electrolyte, and carbon-binder networks. While macrohomogeneous models are often used to predict electrode behavior, accurate predictions remain challenging, owing to the incomplete understanding of the critical role of carbon-binder networks and how they affect the electrochemical response. The present study systematically characterizes these effects in terms of effective properties by utilizing macrohomogeneous models to analyze the measured responses for electrodes with different carbon-binder content, electrode thickness, and porosity but with identical materials. We find that the impact of the carbon-binder network is more severe than previously thought. Even for low carbon-binder content (5 %wt. dry electrode), the presence of the network decreases the reaction area and increases the ion transport resistance, negatively impacting electrode performance. These effects scale with not just porosity or active material volume but also with carbon-binder content. The findings underscore the importance of connecting all effective properties to electrode specifications in a full factorial sense to transform the electrode design paradigm.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1831722

Journal Information:: Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Journal Issue: 7 Vol. 168; ISSN 0013-4651

Publisher:: IOP Publishing - The Electrochemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Influence of Conductive Additives and Binder on the Impedance of Lithium-Ion Battery Electrodes: Effect of Morphology Hein, Simon; Danner, Timo; Westhoff, Daniel Journal of The Electrochemical Society, Vol. 167, Issue 1 https://doi.org/10.1149/1945-7111/ab6b1d	journal	January 2020
Fingerprinting Redox Heterogeneity in Electrodes during Extreme Fast Charging Mistry, Aashutosh; Usseglio-Viretta, Francois L. E.; Colclasure, Andrew Journal of The Electrochemical Society, Vol. 167, Issue 9 https://doi.org/10.1149/1945-7111/ab8fd7	journal	May 2020
Development of Experimental Techniques for Parameterization of Multi-scale Lithium-ion Battery Models Chen, Chang-Hui; Brosa Planella, Ferran; O’Regan, Kieran Journal of The Electrochemical Society, Vol. 167, Issue 8 https://doi.org/10.1149/1945-7111/ab9050	journal	May 2020
Study of the Binder Influence on Expansion/Contraction Behavior of Silicon Alloy Negative Electrodes for Lithium-Ion Batteries Yoon, Dong-Hwan; Marinaro, Mario; Axmann, Peter Journal of The Electrochemical Society, Vol. 167, Issue 16 https://doi.org/10.1149/1945-7111/abcf4f	journal	December 2020
A Dilatometric Study of Graphite Electrodes during Cycling with X-ray Computed Tomography Michael, H.; Iacoviello, F.; Heenan, T. M. M. Journal of The Electrochemical Society, Vol. 168, Issue 1 https://doi.org/10.1149/1945-7111/abd648	journal	January 2021
A Modified Electrochemical Model to Account for Mechanical Effects Due to Lithium Intercalation and External Pressure Zhang, Xiaoxuan; Klinsmann, Markus; Chumakov, Sergei Journal of The Electrochemical Society, Vol. 168, Issue 2 https://doi.org/10.1149/1945-7111/abe16d	journal	February 2021
Editors’ Choice—Quantifying the Impact of Charge Transport Bottlenecks in Composite Cathodes of All-Solid-State Batteries Minnmann, Philip; Quillman, Lars; Burkhardt, Simon Journal of The Electrochemical Society, Vol. 168, Issue 4 https://doi.org/10.1149/1945-7111/abf8d7	journal	April 2021
Quantitative Parameter Estimation, Model Selection, and Variable Selection in Battery Science Brady, Nicholas W.; Gould, Christian Alexander; West, Alan C. Journal of The Electrochemical Society, Vol. 167, Issue 1 https://doi.org/10.1149/2.0012001JES	journal	August 2019
Three-Dimensional Reconstruction of a LiCoO2 Li-Ion Battery Cathode Hutzenlaub, Tobias; Thiele, Simon; Zengerle, Roland Electrochemical and Solid-State Letters, Vol. 15, Issue 3 https://doi.org/10.1149/2.002203esl	journal	January 2012
Computational Model of Magnesium Deposition and Dissolution for Property Determination via Cyclic Voltammetry Chadwick, Alexander F.; Vardar, Gulin; DeWitt, Stephen Journal of The Electrochemical Society, Vol. 163, Issue 9 https://doi.org/10.1149/2.0031609jes	journal	January 2016
Influence of the Active Material on the Electronic Conductivity of the Positive Electrode in Lithium-Ion Batteries Kondo, Hiroki; Sawada, Hiroshi; Okuda, Chikaaki Journal of The Electrochemical Society, Vol. 166, Issue 8 https://doi.org/10.1149/2.0051906jes	journal	January 2019
Method to Determine the In-Plane Tortuosity of Porous Electrodes Suthar, Bharatkumar; Landesfeind, Johannes; Eldiven, Askin Journal of The Electrochemical Society, Vol. 165, Issue 10 https://doi.org/10.1149/2.0121810jes	journal	January 2018
Characterization of Electronic and Ionic Transport in Li _1- _x Ni _0.33 Mn _0.33 Co _0.33 O ₂ (NMC ₃₃₃ ) and Li _1- _x Ni _0.50 Mn _0.20 Co _0.30 O ₂ (NMC ₅₂₃ ) as a Function of Li Content Amin, Ruhul; Chiang, Yet-Ming Journal of The Electrochemical Society, Vol. 163, Issue 8 https://doi.org/10.1149/2.0131608jes	journal	January 2016
Model Based Analysis of One-Dimensional Oriented Lithium-Ion Battery Electrodes Chadha, Tandeep S.; Suthar, Bharatkumar; Rife, Derek Journal of The Electrochemical Society, Vol. 164, Issue 11 https://doi.org/10.1149/2.0141711jes	journal	January 2017
Multiphase Porous Electrode Theory Smith, Raymond B.; Bazant, Martin Z. Journal of The Electrochemical Society, Vol. 164, Issue 11 https://doi.org/10.1149/2.0171711jes	journal	January 2017
Comprehensive Study of the Polarization Behavior of LiFePO ₄ Electrodes Based on a Many-Particle Model Kondo, Hiroki; Sasaki, Tsuyoshi; Barai, Pallab Journal of The Electrochemical Society, Vol. 165, Issue 10 https://doi.org/10.1149/2.0181810jes	journal	January 2018
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
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
Three Dimensional Simulation of Galvanostatic Discharge of LiCoO ₂ Cathode Based on X-ray Nano-CT Images Yan, Bo; Lim, Cheolwoong; Yin, Leilei Journal of The Electrochemical Society, Vol. 159, Issue 10 https://doi.org/10.1149/2.024210jes	journal	January 2012
Discharge Characteristics of Lithium Battery Electrodes with a Semiconducting Polymer Studied by Continuum Modeling and Experiment Wu, Shao-Ling; Javier, Anna E.; Devaux, Didier Journal of The Electrochemical Society, Vol. 161, Issue 12 https://doi.org/10.1149/2.0261412jes	journal	January 2014
Mechanical Degradation of Graphite/PVDF Composite Electrodes: A Model-Experimental Study Takahashi, Kenji; Higa, Kenneth; Mair, Sunil Journal of The Electrochemical Society, Vol. 163, Issue 3 https://doi.org/10.1149/2.0271603jes	journal	December 2015
On Graded Electrode Porosity as a Design Tool for Improving the Energy Density of Batteries Dai, Yiling; Srinivasan, Venkat Journal of The Electrochemical Society, Vol. 163, Issue 3 https://doi.org/10.1149/2.0301603jes	journal	December 2015
Quantifying Inhomogeneity of Lithium Ion Battery Electrodes and Its Influence on Electrochemical Performance Müller, Simon; Eller, Jens; Ebner, Martin Journal of The Electrochemical Society, Vol. 165, Issue 2 https://doi.org/10.1149/2.0311802jes	journal	January 2018
Optimizing Areal Capacities through Understanding the Limitations of Lithium-Ion Electrodes Gallagher, Kevin G.; Trask, Stephen E.; Bauer, Christoph Journal of The Electrochemical Society, Vol. 163, Issue 2 https://doi.org/10.1149/2.0321602jes	journal	November 2015
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
Thermodynamic Model for Substitutional Materials: Application to Lithiated Graphite, Spinel Manganese Oxide, Iron Phosphate, and Layered Nickel-Manganese-Cobalt Oxide Verbrugge, Mark; Baker, Daniel; Koch, Brian Journal of The Electrochemical Society, Vol. 164, Issue 11 https://doi.org/10.1149/2.0341708jes	journal	January 2017
Requirements for Enabling Extreme Fast Charging of High Energy Density Li-Ion Cells while Avoiding Lithium Plating Colclasure, Andrew M.; Dunlop, Alison R.; Trask, Stephen E. Journal of The Electrochemical Society, Vol. 166, Issue 8 https://doi.org/10.1149/2.0451908jes	journal	January 2019
Li-Ion Cell Operation at Low Temperatures Ji, Yan; Zhang, Yancheng; Wang, Chao-Yang Journal of The Electrochemical Society, Vol. 160, Issue 4 https://doi.org/10.1149/2.047304jes	journal	January 2013
Comparing Macroscale and Microscale Simulations of Porous Battery Electrodes Higa, Kenneth; Wu, Shao-Ling; Parkinson, Dilworth Y. Journal of The Electrochemical Society, Vol. 164, Issue 11 https://doi.org/10.1149/2.0501711jes	journal	January 2017
Temperature and Concentration Dependence of the Ionic Transport Properties of Lithium-Ion Battery Electrolytes Landesfeind, Johannes; Gasteiger, Hubert A. Journal of The Electrochemical Society, Vol. 166, Issue 14 https://doi.org/10.1149/2.0571912jes	journal	January 2019
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
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
Quantifying Tortuosity of Porous Li-Ion Battery Electrodes: Comparing Polarization-Interrupt and Blocking-Electrolyte Methods Pouraghajan, Fezzeh; Knight, Hannah; Wray, Michael Journal of The Electrochemical Society, Vol. 165, Issue 11 https://doi.org/10.1149/2.0611811jes	journal	January 2018
Modeling Battery Performance Due to Intercalation Driven Volume Change in Porous Electrodes Garrick, Taylor R.; Higa, Kenneth; Wu, Shao-Ling Journal of The Electrochemical Society, Vol. 164, Issue 11 https://doi.org/10.1149/2.0621711jes	journal	January 2017
High Rate Capability of Li(Ni _1/3 Mn _1/3 Co _1/3 )O ₂ Electrode for Li-Ion Batteries Wu, Shao-Ling; Zhang, Wei; Song, Xiangyun Journal of The Electrochemical Society, Vol. 159, Issue 4 https://doi.org/10.1149/2.062204jes	journal	January 2012
Resolving the Discrepancy in Tortuosity Factor Estimation for Li-Ion Battery Electrodes through Micro-Macro Modeling and Experiment Usseglio-Viretta, Francois L. E.; Colclasure, Andrew; Mistry, Aashutosh N. Journal of The Electrochemical Society, Vol. 165, Issue 14 https://doi.org/10.1149/2.0731814jes	journal	January 2018
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
Fast Impedance Simulation of Lithium-Ion Batteries with Pseudo-Two Dimensional Electrochemical Models Pathak, Manan; Murbach, Matthew D.; Pathak, Chintan Journal of The Electrochemical Society, Vol. 165, Issue 7 https://doi.org/10.1149/2.0831805jes	journal	January 2018
Incorporating Dendrite Growth into Continuum Models of Electrolytes: Insights from NMR Measurements and Inverse Modeling Sethurajan, Athinthra K.; Foster, Jamie M.; Richardson, Giles Journal of The Electrochemical Society, Vol. 166, Issue 8 https://doi.org/10.1149/2.0921908jes	journal	January 2019
Influence of the Binder on Lithium Ion Battery Electrode Tortuosity and Performance Landesfeind, Johannes; Eldiven, Askin; Gasteiger, Hubert A. Journal of The Electrochemical Society, Vol. 165, Issue 5 https://doi.org/10.1149/2.0971805jes	journal	January 2018
Editors' Choice—Mesoscale Analysis of Conductive Binder Domain Morphology in Lithium-Ion Battery Electrodes Trembacki, Bradley L.; Mistry, Aashutosh N.; Noble, David R. Journal of The Electrochemical Society, Vol. 165, Issue 13 https://doi.org/10.1149/2.0981813jes	journal	January 2018
Detection of Binder Gradients Using Impedance Spectroscopy and Their Influence on the Tortuosity of Li-Ion Battery Graphite Electrodes Morasch, Robert; Landesfeind, Johannes; Suthar, Bharatkumar Journal of The Electrochemical Society, Vol. 165, Issue 14 https://doi.org/10.1149/2.1021814jes	journal	January 2018
Is There a Benefit in Employing Graded Electrodes for Lithium-Ion Batteries? Qi, Yanbo; Jang, Taejin; Ramadesigan, Venkatasailanathan Journal of The Electrochemical Society, Vol. 164, Issue 13 https://doi.org/10.1149/2.1051713jes	journal	January 2017
Electroanalytical Methods Utilizing Small Signal Current or Potential Excitations for the Characterization of Porous Electrodes Comprising Insertion Materials Baker, Daniel R.; Verbrugge, Mark W. Journal of The Electrochemical Society, Vol. 160, Issue 8 https://doi.org/10.1149/2.110308jes	journal	January 2013
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
Numerical Prediction of Multiscale Electronic Conductivity of Lithium-Ion Battery Positive Electrodes Cadiou, F.; Etiemble, A.; Douillard, T. Journal of The Electrochemical Society, Vol. 166, Issue 8 https://doi.org/10.1149/2.1221908jes	journal	January 2019
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
Modeling the Effects of Electrode Microstructural Heterogeneities on Li-Ion Battery Performance and Lifetime Forouzan, Mehdi M.; Mazzeo, Brian A.; Wheeler, Dean R. Journal of The Electrochemical Society, Vol. 165, Issue 10 https://doi.org/10.1149/2.1281809jes	journal	January 2018
Galvanostatic Intermittent Titration and Performance Based Analysis of LiNi _0.5 Co _0.2 Mn _0.3 O ₂ Cathode Verma, Ankit; Smith, Kandler; Santhanagopalan, Shriram Journal of The Electrochemical Society, Vol. 164, Issue 13 https://doi.org/10.1149/2.1701713jes	journal	January 2017
Novel microstructure quantification framework for databasing, visualization, and analysis of microstructure data Niezgoda, Stephen R.; Kanjarla, Anand K.; Kalidindi, Surya R. Integrating Materials and Manufacturing Innovation, Vol. 2, Issue 1 https://doi.org/10.1186/2193-9772-2-3	journal	July 2013

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