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.
Ferraro, Mark Edward, et al. "Electrode Mesoscale as a Collection of Particles: Coupled Electrochemical and Mechanical Analysis of NMC Cathodes." Journal of the Electrochemical Society (Online), vol. 167, no. 1, Dec. 2019. https://doi.org/10.1149/1945-7111/ab632b
Ferraro, Mark Edward, Trembacki, Bradley, Brunini, Victor, Noble, David R., & Roberts, Scott Alan (2019). Electrode Mesoscale as a Collection of Particles: Coupled Electrochemical and Mechanical Analysis of NMC Cathodes. Journal of the Electrochemical Society (Online), 167(1). https://doi.org/10.1149/1945-7111/ab632b
Ferraro, Mark Edward, Trembacki, Bradley, Brunini, Victor, et al., "Electrode Mesoscale as a Collection of Particles: Coupled Electrochemical and Mechanical Analysis of NMC Cathodes," Journal of the Electrochemical Society (Online) 167, no. 1 (2019), https://doi.org/10.1149/1945-7111/ab632b
@article{osti_1605733,
author = {Ferraro, Mark Edward and Trembacki, Bradley and Brunini, Victor and Noble, David R. and Roberts, Scott Alan},
title = {Electrode Mesoscale as a Collection of Particles: Coupled Electrochemical and Mechanical Analysis of NMC Cathodes},
annote = {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.},
doi = {10.1149/1945-7111/ab632b},
url = {https://www.osti.gov/biblio/1605733},
journal = {Journal of the Electrochemical Society (Online)},
issn = {ISSN 1945-7111},
number = {1},
volume = {167},
place = {United States},
publisher = {IOP Publishing},
year = {2019},
month = {12}}
Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States); Sandia National Laboratories (SNL-CA), Livermore, CA (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Program (EE-2G)
Grant/Contract Number:
AC04-94AL85000
OSTI ID:
1605733
Report Number(s):
SAND--2020-2283J; 684143
Journal Information:
Journal of the Electrochemical Society (Online), Journal Name: Journal of the Electrochemical Society (Online) Journal Issue: 1 Vol. 167; ISSN 1945-7111