skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Electrode Mesoscale as a Collection of Particles: Coupled Electrochemical and Mechanical Analysis of NMC Cathodes

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

Battery electrodes are composed of polydisperse particles and a porous, composite binder domain. These materials are arranged into a complex mesostructure whose morphology impacts both electrochemical performance and mechanical response. We present image-based, particle-resolved, mesoscale finite element model simulations of coupled electrochemical-mechanical performance on a representative NMC electrode domain. Beyond predicting macroscale quantities such as half-cell voltage and evolving electrical conductivity, studying behaviors on a per-particle and per-surface basis enables performance and material design insights previously unachievable. Voltage losses are primarily attributable to a complex interplay between interfacial charge transfer kinetics, lithium diffusion, and, locally, electrical conductivity. Mesoscale heterogeneities arise from particle polydispersity and lead to material underutilization at high current densities. Particle-particle contacts, however, reduce heterogeneities by enabling lithium diffusion between connected particle groups. While the porous composite binder domain (CBD) may have slower ionic transport and less available area for electrochemical reactions, its high electrical conductivity makes it the preferred reaction site late in electrode discharge. Mesoscale results are favorably compared to both experimental data and macrohomogeneous models. This work enables improvements in materials design by providing a tool for optimization of particle sizes, CBD morphology, and manufacturing conditions.

Research Organization:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Vehicle Technologies Office (VTO)
Grant/Contract Number:
AC04-94AL85000
OSTI ID:
1605733
Report Number(s):
SAND-2020-2283J; 684143
Journal Information:
Journal of the Electrochemical Society (Online), Vol. 167, Issue 1; ISSN 1945-7111
Publisher:
IOP PublishingCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 57 works
Citation information provided by
Web of Science

References (101)

Electrochemomechanical performance of porous electrode incorporating binder network journal July 2019
Binder effect on cycling performance of silicon/carbon composite anodes for lithium ion batteries journal August 2006
Three-Dimensional Visualization of Conductive Domains in Battery Electrodes with Contrast-Enhancing Nanoparticles journal September 2018
Editors' Choice—Mesoscale Analysis of Conductive Binder Domain Morphology in Lithium-Ion Battery Electrodes journal January 2018
Modeling 3D Microstructure and Ion Transport in Porous Li-Ion Battery Electrodes journal January 2011
Three-dimensional finite element study on stress generation in synchrotron X-ray tomography reconstructed nickel-manganese-cobalt based half cell journal December 2016
Mesoscale Electrochemical Performance Simulation of 3D Interpenetrating Lithium-Ion Battery Electrodes journal January 2019
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
Lithium ion battery electrodes predicted from manufacturing simulations: Assessing the impact of the carbon-binder spatial location on the electrochemical performance journal December 2019
A Framework for Three-Dimensional Mesoscale Modeling of Anisotropic Swelling and Mechanical Deformation in Lithium-Ion Electrodes journal January 2014
Transport-Geometry Interactions in Li-Ion Cathode Materials Imaged Using X-ray Nanotomography journal January 2017
Semianalytical study of the effect of realistic boundary conditions on diffusion induced stresses in cylindrical lithium ion electrode-binder system journal November 2019
Stochastic microstructure modeling and electrochemical simulation of lithium-ion cell anodes in 3D journal December 2016
A conformal decomposition finite element method for modeling stationary fluid interface problems journal January 2009
Electrode microstructure controls localized electronic impedance in Li-ion batteries journal February 2019
Resolving the Discrepancy in Tortuosity Factor Estimation for Li-Ion Battery Electrodes through Micro-Macro Modeling and Experiment journal January 2018
Lithium ion rechargeable batteries: State of the art and future needs of microscopic theoretical models and simulations journal February 2015
A particle-resolved 3D finite element model to study the effect of cathode microstructure on the behavior of lithium ion batteries journal January 2019
Using Synchrotron X-Ray Nano-CT to Characterize SOFC Electrode Microstructures in Three-Dimensions at Operating Temperature journal January 2011
X-Ray Tomography of Porous, Transition Metal Oxide Based Lithium Ion Battery Electrodes journal March 2013
Nanoscale X-ray imaging of ageing in automotive lithium ion battery cells journal September 2019
Morphology of nanoporous carbon-binder domains in Li-ion batteries—A FIB-SEM study journal November 2015
A Modified Multiphysics model for Lithium-Ion batteries with a LixNi1/3Mn1/3Co1/3O2 electrode journal August 2015
Determining the uncertainty in microstructural parameters extracted from tomographic data journal January 2018
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
Modeling the effect of electrode thickness on the performance of lithium-ion batteries with experimental validation journal November 2019
Characterization of the 3-dimensional microstructure of a graphite negative electrode from a Li-ion battery journal March 2010
Simulation of diffusion-induced stress using reconstructed electrodes particle structures generated by micro/nano-CT journal July 2012
Micro-Macroscopic Coupled Modeling of Batteries and Fuel Cells journal January 1998
A review on lithium-ion battery ageing mechanisms and estimations for automotive applications journal November 2013
Ageing mechanisms in lithium-ion batteries journal September 2005
Manufacturing Process for Improved Ultra‐Thick Cathodes in High‐Energy Lithium‐Ion Batteries journal June 2019
Disintegration of Meatball Electrodes for LiNi x Mn y Co z O2 Cathode Materials journal May 2017
Influence of the Carbon Black Dispersing Process on the Microstructure and Performance of Li‐Ion Battery Cathodes journal June 2019
Comparison of Modeling Predictions with Experimental Data from Plastic Lithium Ion Cells journal January 1996
Mesoscale Effective Property Simulations Incorporating Conductive Binder journal January 2017
Heterogeneous damage in Li-ion batteries: Experimental analysis and theoretical modeling journal August 2019
Transport Properties of LiPF[sub 6]-Based Li-Ion Battery Electrolytes journal January 2005
Three-dimensional electrochemical Li-ion battery modelling featuring a focused ion-beam/scanning electron microscopy based three-phase reconstruction of a LiCoO2 cathode journal January 2014
Effects of Various Conductive Additive and Polymeric Binder Contents on the Performance of a Lithium-Ion Composite Cathode journal January 2008
Three-dimensional investigation of cycling-induced microstructural changes in lithium-ion battery cathodes using focused ion beam/scanning electron microscopy journal February 2016
Effects of three-dimensional cathode microstructure on the performance of lithium-ion battery cathodes journal January 2013
Rethinking How External Pressure Can Suppress Dendrites in Lithium Metal Batteries journal January 2019
A Computational Model of the Mechanical Behavior within Reconstructed LixCoO2 Li-ion Battery Cathode Particles journal June 2014
Berechnung verschiedener physikalischer Konstanten von heterogenen Substanzen. I. Dielektrizitätskonstanten und Leitfähigkeiten der Mischkörper aus isotropen Substanzen journal January 1935
A new open computational framework for highly-resolved coupled three-dimensional multiphysics simulations of Li-ion cells journal January 2014
Joint structural and electrochemical modeling: Impact of porosity on lithium-ion battery performance journal August 2019
Electro-chemo-mechanical simulation for lithium ion batteries across the scales journal February 2020
Visualizing the Carbon Binder Phase of Battery Electrodes in Three Dimensions journal July 2018
Quantification and modeling of mechanical degradation in lithium-ion batteries based on nanoscale imaging journal June 2018
Impact of External Pressure and Electrolyte Transport Properties on Lithium Dendrite Growth journal January 2018
Kinetics of Materials book September 2005
Grid indentation analysis of mechanical properties of composite electrodes in Li-ion batteries journal December 2016
Probing the Role of Electrode Microstructure in the Lithium-Ion Battery Thermal Behavior journal January 2017
Swelling and softening of lithium-ion battery separators in electrolyte solvents journal October 2015
Investigation of binder distribution in graphite anodes for lithium-ion batteries journal February 2017
Comparing Macroscale and Microscale Simulations of Porous Battery Electrodes journal January 2017
Three-Phase Multiscale Modeling of a LiCoO 2 Cathode: Combining the Advantages of FIB-SEM Imaging and X-Ray Tomography journal November 2014
Investigation of film solidification and binder migration during drying of Li-Ion battery anodes journal June 2016
Lithiation-Induced Dilation Mapping in a Lithium-Ion Battery Electrode by 3D X-Ray Microscopy and Digital Volume Correlation journal November 2013
In-Situ Nanoindentation Measurement of Local Mechanical Behavior of a Li-Ion Battery Cathode in Liquid Electrolyte journal November 2018
Three Dimensional Simulation of Galvanostatic Discharge of LiCoO 2 Cathode Based on X-ray Nano-CT Images journal January 2012
Visualization and Quantification of Electrochemical and Mechanical Degradation in Li Ion Batteries journal October 2013
A consistently coupled multiscale mechanical–electrochemical battery model with particle interaction and its validation journal April 2019
Vegard’s law journal March 1991
Electrochemical and Physical Properties of Ti-Substituted Layered Nickel Manganese Cobalt Oxide (NMC) Cathode Materials journal January 2012
Geometric Characteristics of Three Dimensional Reconstructed Anode Electrodes of Lithium Ion Batteries journal April 2014
A conformal decomposition finite element method for arbitrary discontinuities on moving interfaces: CDFEM FOR ARBITRARY DISCONTINUITIES ON MOVING INTERFACES journal June 2014
Conductivity Degradation of Polyvinylidene Fluoride Composite Binder during Cycling: Measurements and Simulations for Lithium-Ion Batteries journal January 2016
Solid-state diffusion limitations on pulse operation of a lithium ion cell for hybrid electric vehicles journal October 2006
Influence of the Binder on Lithium Ion Battery Electrode Tortuosity and Performance journal January 2018
Micro-Scale Modeling of Li-Ion Batteries: Parameterization and Validation journal January 2012
A verified conformal decomposition finite element method for implicit, many-material geometries journal December 2018
Mesoscale Effects of Composition and Calendering in Lithium-Ion Battery Composite Electrodes
  • Trembacki, Bradley L.; Noble, David R.; Ferraro, Mark E.
  • Journal of Electrochemical Energy Conversion and Storage, Vol. 17, Issue 4 https://doi.org/10.1115/1.4045973
journal March 2020
Effects of Inhomogeneities—Nanoscale to Mesoscale—on the Durability of Li-Ion Batteries journal February 2013
Correlation of Electrolyte Volume and Electrochemical Performance in Lithium-Ion Pouch Cells with Graphite Anodes and NMC532 Cathodes journal January 2017
Critical Role of Polymeric Binders on the Electronic Transport Properties of Composites Electrode journal January 2006
Mesoscale modeling in electrochemical devices—A critical perspective journal March 2019
Particles and Polymer Binder Interaction: A Controlling Factor in Lithium-Ion Electrode Performance journal January 2012
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 journal January 2016
A three-dimensional meso-macroscopic model for Li-Ion intercalation batteries journal September 2016
Modeling of Galvanostatic Charge and Discharge of the Lithium/Polymer/Insertion Cell journal January 1993
Numerical Simulation of Intercalation-Induced Stress in Li-Ion Battery Electrode Particles journal January 2007
X-Ray Tomography for Lithium Ion Battery Research: A Practical Guide journal July 2017
Intercalation-Induced Stress and Heat Generation within Single Lithium-Ion Battery Cathode Particles journal January 2008
3D analysis of a LiCoO2–Li(Ni1/3Mn1/3Co1/3)O2 Li-ion battery positive electrode using x-ray nano-tomography journal March 2013
A Combination of X-Ray Tomography and Carbon Binder Modeling: Reconstructing the Three Phases of LiCoO 2 Li-Ion Battery Cathodes journal January 2014
Understanding the Degradation Mechanisms of LiNi 0.5 Co 0.2 Mn 0.3 O 2 Cathode Material in Lithium Ion Batteries journal August 2013
Three-Phase 3D Reconstruction of a LiCoO 2 Cathode via FIB-SEM Tomography journal January 2016
Modeling of contact stress among compound particles in high energy lithium-ion battery journal March 2019
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) journal March 2017
A Boundary Condition for Porous Electrodes journal January 2004
Numerical Simulation of Stress Evolution in Lithium Manganese Dioxide Particles due to Coupled Phase Transition and Intercalation journal January 2011
Multiple imaging mode X-ray computed tomography for distinguishing active and inactive phases in lithium-ion battery cathodes journal June 2015
Mechanical and Electrochemical Response of a LiCoO2 Cathode using Reconstructed Microstructures journal February 2016
Secondary-Phase Stochastics in Lithium-Ion Battery Electrodes journal January 2018
The effect of binders on the rheological properties and the microstructure formation of lithium-ion battery anode slurries journal December 2015
Numerical Prediction of Multiscale Electronic Conductivity of Lithium-Ion Battery Positive Electrodes journal January 2019
Main aging mechanisms in Li ion batteries journal August 2005
Three-Dimensional Reconstruction of a LiCoO2 Li-Ion Battery Cathode journal January 2012
High Rate Capability of Li(Ni 1/3 Mn 1/3 Co 1/3 )O 2 Electrode for Li-Ion Batteries journal January 2012

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:1605733

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 · OSTI ID:1605733

Mesoscale Effective Property Simulations Incorporating Conductive Binder
Journal Article · Wed Jul 26 00:00:00 EDT 2017 · Journal of the Electrochemical Society · OSTI ID:1605733

Related Subjects