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

Title: Secondary-Phase Stochastics in Lithium-Ion Battery Electrodes

Abstract

Lithium-ion battery electrodes exhibit complex interplay among multiple electrochemically coupled transport processes, which rely on the underlying functionality and relative arrangement of different constituent phases. The electrochemically inactive solid phases (e.g., conductive additive and binder, referred to as the secondary phase), while beneficial for improved electronic conductivity and mechanical integrity, may partially block the electrochemically active sites and introduce additional transport resistances in the pore (electrolyte) phase. In this work, the role of mesoscale interactions and inherent stochasticity in porous electrodes is elucidated in the context of short-range (interface) and long-range (transport) characteristics. The electrode microstructure significantly affects kinetically and transport-limiting scenarios and thereby the cell performance. The secondary-phase morphology is also found to strongly influence the microstructure-transport-kinetics interactions. Apropos, strategies have been proposed for performance improvement via electrode microstructural modifications.

Authors:
 [1];  [2]; ORCiD logo [1]
  1. Purdue Univ., West Lafayette, IN (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1419417
Report Number(s):
NREL/JA-5400-70743
Journal ID: ISSN 1944-8244
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 10; Journal Issue: 7; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; conductive binder; electrochemically active area; electrode microstructural characterization; Li-ion battery; porous composite electrode; secondary-phase morphology

Citation Formats

Mistry, Aashutosh N., Smith, Kandler, and Mukherjee, Partha P. Secondary-Phase Stochastics in Lithium-Ion Battery Electrodes. United States: N. p., 2018. Web. doi:10.1021/acsami.7b17771.
Mistry, Aashutosh N., Smith, Kandler, & Mukherjee, Partha P. Secondary-Phase Stochastics in Lithium-Ion Battery Electrodes. United States. https://doi.org/10.1021/acsami.7b17771
Mistry, Aashutosh N., Smith, Kandler, and Mukherjee, Partha P. 2018. "Secondary-Phase Stochastics in Lithium-Ion Battery Electrodes". United States. https://doi.org/10.1021/acsami.7b17771. https://www.osti.gov/servlets/purl/1419417.
@article{osti_1419417,
title = {Secondary-Phase Stochastics in Lithium-Ion Battery Electrodes},
author = {Mistry, Aashutosh N. and Smith, Kandler and Mukherjee, Partha P.},
abstractNote = {Lithium-ion battery electrodes exhibit complex interplay among multiple electrochemically coupled transport processes, which rely on the underlying functionality and relative arrangement of different constituent phases. The electrochemically inactive solid phases (e.g., conductive additive and binder, referred to as the secondary phase), while beneficial for improved electronic conductivity and mechanical integrity, may partially block the electrochemically active sites and introduce additional transport resistances in the pore (electrolyte) phase. In this work, the role of mesoscale interactions and inherent stochasticity in porous electrodes is elucidated in the context of short-range (interface) and long-range (transport) characteristics. The electrode microstructure significantly affects kinetically and transport-limiting scenarios and thereby the cell performance. The secondary-phase morphology is also found to strongly influence the microstructure-transport-kinetics interactions. Apropos, strategies have been proposed for performance improvement via electrode microstructural modifications.},
doi = {10.1021/acsami.7b17771},
url = {https://www.osti.gov/biblio/1419417}, journal = {ACS Applied Materials and Interfaces},
issn = {1944-8244},
number = 7,
volume = 10,
place = {United States},
year = {Fri Jan 12 00:00:00 EST 2018},
month = {Fri Jan 12 00:00:00 EST 2018}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 95 works
Citation information provided by
Web of Science

Figures / Tables:

Figure 1 Figure 1: (a) Composite cathode for LIBs is made up of multiple phases: AM particles, conductive additives, binder, and voids for ionic transport. (b) Given the order of magnitude difference in length scales of conductive additives and AM, the distribution of conductive additives + binder (referred to as secondary phasemore » or carbon binder domain) can be jointly expressed as a homogeneous phase. (c−e) The microstructure generation procedure outlined here grows the secondary phase with different morphologies varying between a film-type structure (ω = 0) and a fingerlike arrangement (ω = 1). Also, going toward higher morphologies (i.e., ω→ 1) gives rise to a secondary pore network with a smaller pore size in thicker carbon binder domains.« less

Save / Share:

Works referenced in this record:

Nonaqueous Liquid Electrolytes for Lithium-Based Rechargeable Batteries
journal, October 2004


Electrochemistry and the Future of the Automobile
journal, June 2010


Materials Challenges and Opportunities of Lithium Ion Batteries
journal, January 2011


Challenges in the development of advanced Li-ion batteries: a review
journal, January 2011


Electrolytes and Interphases in Li-Ion Batteries and Beyond
journal, October 2014


New Horizons for Conventional Lithium Ion Battery Technology
journal, September 2014


Prospects and Limits of Energy Storage in Batteries
journal, February 2015


Ageing mechanisms in lithium-ion batteries
journal, September 2005


Building better batteries
journal, February 2008


Chemistry, Impedance, and Morphology Evolution in Solid Electrolyte Interphase Films during Formation in Lithium Ion Batteries
journal, December 2013


Effects of Inhomogeneities—Nanoscale to Mesoscale—on the Durability of Li-Ion Batteries
journal, February 2013


Issues and challenges facing rechargeable lithium batteries
journal, November 2001


A General Discussion of Li Ion Battery Safety
journal, January 2012


The Li-Ion Rechargeable Battery: A Perspective
journal, January 2013


Positive Electrode Materials for Li-Ion and Li-Batteries
journal, February 2010


Alloy Negative Electrodes for Li-Ion Batteries
journal, October 2014


Effects of Various Conductive Additive and Polymeric Binder Contents on the Performance of a Lithium-Ion Composite Cathode
journal, January 2008


Cooperation between Active Material, Polymeric Binder and Conductive Carbon Additive in Lithium Ion Battery Cathode
journal, February 2012


Particles and Polymer Binder Interaction: A Controlling Factor in Lithium-Ion Electrode Performance
journal, January 2012


Electrochemical Properties of LiCoO 2 Electrodes with Latex Binders on High-Voltage Exposure
journal, January 2015


Conveying Advanced Li-ion Battery Materials into Practice The Impact of Electrode Slurry Preparation Skills
journal, July 2016


Mechanistic Understanding of the Role of Evaporation in Electrode Processing
journal, January 2017


The Morphology of Battery Electrodes with the Focus of the Conductive Additives Paths
journal, January 2015


Three-dimensional microstructural imaging methods for energy materials
journal, January 2013


Characterization of the 3-dimensional microstructure of a graphite negative electrode from a Li-ion battery
journal, March 2010


Measurement of three-dimensional microstructure in a LiCoO2 positive electrode
journal, April 2011


Multi Length Scale Microstructural Investigations of a Commercially Available Li-Ion Battery Electrode
journal, January 2012


Quantitative Characterization of LiFePO 4 Cathodes Reconstructed by FIB/SEM Tomography
journal, January 2012


3D analysis of a LiCoO2–Li(Ni1/3Mn1/3Co1/3)O2 Li-ion battery positive electrode using x-ray nano-tomography
journal, March 2013


Visualization and Quantification of Electrochemical and Mechanical Degradation in Li Ion Batteries
journal, October 2013


X-Ray Tomography of Porous, Transition Metal Oxide Based Lithium Ion Battery Electrodes
journal, March 2013


The application of phase contrast X-ray techniques for imaging Li-ion battery electrodes
journal, April 2014


Modeling of Galvanostatic Charge and Discharge of the Lithium/Polymer/Insertion Cell
journal, January 1993


Optimizing Areal Capacities through Understanding the Limitations of Lithium-Ion Electrodes
journal, November 2015


Thick electrodes for Li-ion batteries: A model based analysis
journal, December 2016


Tortuosity Anisotropy in Lithium-Ion Battery Electrodes
journal, October 2013


Tool for Tortuosity Estimation in Lithium Ion Battery Porous Electrodes
journal, December 2014


The Effect of Microstructure on the Galvanostatic Discharge of Graphite Anode Electrodes in LiCoO[sub 2]-Based Rocking-Chair Rechargeable Batteries
journal, January 2009


Mechanical and Electrochemical Response of a LiCoO2 Cathode using Reconstructed Microstructures
journal, February 2016


Microstructural effects on the average properties in porous battery electrodes
journal, March 2016


Mesoscale Effective Property Simulations Incorporating Conductive Binder
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


A Combination of X-Ray Tomography and Carbon Binder Modeling: Reconstructing the Three Phases of LiCoO 2 Li-Ion Battery Cathodes
journal, January 2014


Analysis of Long-Range Interaction in Lithium-Ion Battery Electrodes
journal, August 2016

  • 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

Mesoscale Elucidation of the Influence of Mixing Sequence in Electrode Processing
journal, December 2014


Microstructure Evolution in Lithium-Ion Battery Electrode Processing
journal, January 2014


Transport Properties of LiPF[sub 6]-Based Li-Ion Battery Electrolytes
journal, January 2005


Works referencing / citing this record:

Volume-Averaged Electrochemical Performance Modeling of 3D Interpenetrating Battery Electrode Architectures
journal, September 2019


Numerical Prediction of Multiscale Electronic Conductivity of Lithium-Ion Battery Positive Electrodes
journal, January 2019


Perspective—Mesoscale Physics in the Catalyst Layer of Proton Exchange Membrane Fuel Cells
journal, January 2019


Mesoscale Electrochemical Performance Simulation of 3D Interpenetrating Lithium-Ion Battery Electrodes
journal, January 2019


Modeling and Simulation of Pore Morphology Modifications using Laser-Structured Graphite Anodes in Lithium-Ion Batteries
journal, September 2019


Probing spatial coupling of resistive modes in porous intercalation electrodes through impedance spectroscopy
journal, January 2019


Non-equilibrium thermodynamics in electrochemical complexation of Li–oxygen porous electrodes
journal, January 2019


Deconstructing electrode pore network to learn transport distortion
journal, December 2019


Editors' Choice—Mesoscale Analysis of Conductive Binder Domain Morphology in Lithium-Ion Battery Electrodes
journal, January 2018


Quantifying the unknown impact of segmentation uncertainty on image-based simulations
text, January 2020


Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.