Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Probing the Role of Multi-scale Heterogeneity in Graphite Electrodes for Extreme Fast Charging

Journal Article · · ACS Applied Materials and Interfaces

Electrode-scale heterogeneity can combine with complex electrochemical interactions to impede lithium-ion battery performance, particularly during fast charging. This research investigates the influence of electrode heterogeneity at different scales on the lithium-ion battery electrochemical performance under operational extremes. We employ image-based mesoscale simulation in conjunction with a three-dimensional electrochemical model to predict performance variability in 14 graphite electrode X-ray computed tomography data sets. Our analysis reveals that the tortuous anisotropy stemming from the variable particle morphology has a dominating influence on the overall cell performance. Cells with platelet morphology achieve lower capacity, higher heat generation rates, and severe plating under extreme fast charge conditions. On the contrary, the heterogeneity due to the active material clustering alone has minimal impact. Our work suggests that manufacturing electrodes with more homogeneous and isotropic particle morphology will improve electrochemical performance and improve safety, enabling electromobility.

Research Organization:
Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program
Grant/Contract Number:
NA0003525
OSTI ID:
1870491
Report Number(s):
SAND2022-4741J; 705122
Journal Information:
ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 16 Vol. 14; ISSN 1944-8244
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (69)

Local State-of-Charge Mapping of Lithium-Ion Battery Electrodes journal July 2011
Tortuosity Anisotropy in Lithium-Ion Battery Electrodes journal October 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
Three-Phase Multiscale Modeling of a LiCoO 2 Cathode: Combining the Advantages of FIB-SEM Imaging and X-Ray Tomography journal November 2014
Quantification of Heterogeneous Degradation in Li‐Ion Batteries journal May 2019
Berechnung verschiedener physikalischer Konstanten von heterogenen Substanzen. III. Die elastischen Konstanten der quasiisotropen Mischkörper aus isotropen Substanzen journal January 1937
Interplay of Lithium Intercalation and Plating on a Single Graphite Particle journal February 2021
Nondestructive detection, characterization, and quantification of lithium plating in commercial lithium-ion batteries journal May 2014
Lithium plating in lithium-ion batteries investigated by voltage relaxation and in situ neutron diffraction journal February 2017
Abuse behavior of high-power, lithium-ion cells journal January 2003
BoneJ: Free and extensible bone image analysis in ImageJ journal December 2010
Effects of three-dimensional cathode microstructure on the performance of lithium-ion battery cathodes journal January 2013
Mechanical and Electrochemical Response of a LiCoO2 Cathode using Reconstructed Microstructures journal February 2016
Enabling fast charging of lithium-ion batteries through secondary-/dual- pore network: Part II - numerical model journal May 2020
Enabling fast charging of lithium-ion batteries through secondary- /dual- pore network: Part I - Analytical diffusion model journal May 2020
Electrode manufacturing for lithium-ion batteries—Analysis of current and next generation processing journal October 2019
A verified conformal decomposition finite element method for implicit, many-material geometries journal December 2018
Image based modelling of microstructural heterogeneity in LiFePO 4 electrodes for Li-ion batteries journal February 2014
Lithium plating in a commercial lithium-ion battery – A low-temperature aging study journal February 2015
Multiple imaging mode X-ray computed tomography for distinguishing active and inactive phases in lithium-ion battery cathodes journal June 2015
Multiscale modeling of lithium-ion battery electrodes based on nano-scale X-ray computed tomography journal March 2016
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
Understanding the trilemma of fast charging, energy density and cycle life of lithium-ion batteries journal October 2018
Lithium ion battery electrodes predicted from manufacturing simulations: Assessing the impact of the carbon-binder spatial location on the electrochemical performance journal December 2019
Spatially Resolving Lithiation in Silicon–Graphite Composite Electrodes via in Situ High-Energy X-ray Diffraction Computed Tomography journal April 2019
Three-Dimensional Visualization of Conductive Domains in Battery Electrodes with Contrast-Enhancing Nanoparticles journal September 2018
In Operando Detection of the Onset and Mapping of Lithium Plating Regimes during Fast Charging of Lithium-Ion Batteries journal June 2020
Controlling Binder Adhesion to Impact Electrode Mesostructures and Transport journal July 2020
Probing the Influence of Multiscale Heterogeneity on Effective Properties of Graphite Electrodes journal January 2022
Secondary-Phase Stochastics in Lithium-Ion Battery Electrodes journal January 2018
Electrochemistry Coupled Mesoscale Complexations in Electrodes Lead to Thermo-Electrochemical Extremes journal August 2018
Stochasticity at Scales Leads to Lithium Intercalation Cascade journal March 2020
Cooperation between Active Material, Polymeric Binder and Conductive Carbon Additive in Lithium Ion Battery Cathode journal February 2012
Effects of Inhomogeneities—Nanoscale to Mesoscale—on the Durability of Li-Ion Batteries journal February 2013
Visualization of Charge Distribution in a Lithium Battery Electrode journal June 2010
Promise and reality of post-lithium-ion batteries with high energy densities journal March 2016
3D microstructure design of lithium-ion battery electrodes assisted by X-ray nano-computed tomography and modelling journal April 2020
Pores for thought: generative adversarial networks for stochastic reconstruction of 3D multi-phase electrode microstructures with periodic boundaries journal June 2020
Challenges and opportunities towards fast-charging battery materials journal June 2019
Visualizing the chemistry and structure dynamics in lithium-ion batteries by in-situ neutron diffraction journal October 2012
Homogeneity of lithium distribution in cylinder-type Li-ion batteries journal December 2015
Sustainable transportation based on electric vehicle concepts: a brief overview journal January 2010
Determining the uncertainty in microstructural parameters extracted from tomographic data journal January 2018
Quantifying lithium concentration gradients in the graphite electrode of Li-ion cells using operando energy dispersive X-ray diffraction journal January 2019
In operando signature and quantification of lithium plating 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
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
Comparison of Modeling Predictions with Experimental Data from Plastic Lithium Ion Cells journal January 1996
Modeling a Porous Intercalation Electrode with Two Characteristic Particle Sizes journal January 1997
Modeling of Galvanostatic Charge and Discharge of the Lithium/Polymer/Insertion Cell journal January 1993
A Critical Review of Thermal Issues in Lithium-Ion Batteries journal January 2011
Fast Charging of Lithium-ion Batteries via Electrode Engineering journal January 2020
Fingerprinting Redox Heterogeneity in Electrodes during Extreme Fast Charging journal May 2020
Quantitative Relationships Between Pore Tortuosity, Pore Topology, and Solid Particle Morphology Using a Novel Discrete Particle Size Algorithm journal June 2020
Tool for Tortuosity Estimation in Lithium Ion Battery Porous Electrodes journal December 2014
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
Bruggeman's Exponents for Effective Thermal Conductivity of Lithium-Ion Battery Electrodes journal November 2015
Review—Electromobility: Batteries or Fuel Cells? journal January 2015
Tortuosity of Battery Electrodes: Validation of Impedance-Derived Values and Critical Comparison with 3D Tomography journal January 2018
Quantifying Inhomogeneity of Lithium Ion Battery Electrodes and Its Influence on Electrochemical Performance journal January 2018
Requirements for Enabling Extreme Fast Charging of High Energy Density Li-Ion Cells while Avoiding Lithium Plating journal January 2019
Interplay of Operational Parameters on Lithium Deposition in Lithium-Ion Cells: Systematic Measurements with Reconstructed 3-Electrode Pouch Full Cells journal January 2016
Mesoscale Effective Property Simulations Incorporating Conductive Binder journal January 2017
In-Situ Detection of Lithium Plating Using High Precision Coulometry journal January 2015
Resolving the Discrepancy in Tortuosity Factor Estimation for Li-Ion Battery Electrodes through Micro-Macro Modeling and Experiment journal January 2018
Extreme Fast Charge Challenges for Lithium-Ion Battery: Variability and Positive Electrode Issues journal January 2019
Editors' Choice—Mesoscale Analysis of Conductive Binder Domain Morphology in Lithium-Ion Battery Electrodes journal January 2018
Mechanistic Understanding of the Role of Evaporation in Electrode Processing journal January 2017
Degradation Diagnostics for Commercial Lithium-Ion Cells Tested at − 10°C journal January 2017

Similar Records

Probing the Influence of Multiscale Heterogeneity on Effective Properties of Graphite Electrodes
Journal Article · Sun Jan 02 23:00:00 EST 2022 · ACS Applied Materials and Interfaces · OSTI ID:1841994

Understanding Impact of Local Heterogeneities During Fast Charge
Conference · Mon Jul 22 00:00:00 EDT 2019 · OSTI ID:1545267

Quantification of Heterogeneous Degradation in Li-Ion Batteries
Journal Article · Tue May 28 00:00:00 EDT 2019 · Advanced Energy Materials · OSTI ID:1524198