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Title: Methodologies for Design, Characterization and Testing of Electrolytes that Enable Extreme Fast Charging of Lithium-ion Cells

Abstract

Selection, testing and validation of electrolyte candidates for Li-ion cells are discussed, based on a 10-minute target for extreme fast charge (XFC). A combination of modeling and laboratory measurements create a timely and synergistic approach to identifying candidate electrolyte formulations. Multi-solvent systems provide a balanced set of properties, wherein lower molecular-weight solvents offer reduced viscosity, increased species diffusivity, and mitigation of concentration polarization at high charge rates. Carefully selected formulations can exhibit peak conductivity and usable conductivity range of two to three times that of the baseline EC-EMC (3:7, wt.) + LiPF6. Candidates are also chosen based on stability and longevity within the cell environment. Lab testing coincides with property predictions from the Advanced Electrolyte Model (AEM) and a macro-scale cell model. Furthermore, cell testing utilized coin and pouch cells having NMC532 or NMC811 cathodes with graphite electrodes. Results indicate combinations of low-molecular weight solvents are key for fast-charge electrolytes as they extend the useful conductivity range to both low and higher salt concentrations, and possess higher self-diffusivities compared to conventional solvents. This reduces impacts from concentration polarization. The choice of electrolyte also influences the tendency for lithium metal deposition at the anode, as showcased by experimental and modeling resultsmore » herein.« less

Authors:
 [1];  [1];  [1];  [1];  [2];  [3];  [3];  [3];  [3];  [3];  [1]
  1. Idaho National Lab. (INL), Idaho Falls, ID (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  3. Argonne National Lab. (ANL), Lemont, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1840534
Alternate Identifier(s):
OSTI ID: 1829377
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Energy Storage Materials
Additional Journal Information:
Journal Volume: 44; Journal ID: ISSN 2405-8297
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; advanced electrolyte model (AEM); cell transport model; extreme fast charge; lithium metal plating; lithium-ion batteries

Citation Formats

Gao, Ningshengjie, Kim, Sangwook, Chinnam, Parameswara, Dufek, Eric J., Colclasure, Andrew M., Jansen, Andrew, Son, Seoung-Bum, Bloom, Ira, Dunlop, Alison, Trask, Stephen, and Gering, Kevin L. Methodologies for Design, Characterization and Testing of Electrolytes that Enable Extreme Fast Charging of Lithium-ion Cells. United States: N. p., 2021. Web. doi:10.1016/j.ensm.2021.10.011.
Gao, Ningshengjie, Kim, Sangwook, Chinnam, Parameswara, Dufek, Eric J., Colclasure, Andrew M., Jansen, Andrew, Son, Seoung-Bum, Bloom, Ira, Dunlop, Alison, Trask, Stephen, & Gering, Kevin L. Methodologies for Design, Characterization and Testing of Electrolytes that Enable Extreme Fast Charging of Lithium-ion Cells. United States. https://doi.org/10.1016/j.ensm.2021.10.011
Gao, Ningshengjie, Kim, Sangwook, Chinnam, Parameswara, Dufek, Eric J., Colclasure, Andrew M., Jansen, Andrew, Son, Seoung-Bum, Bloom, Ira, Dunlop, Alison, Trask, Stephen, and Gering, Kevin L. Sat . "Methodologies for Design, Characterization and Testing of Electrolytes that Enable Extreme Fast Charging of Lithium-ion Cells". United States. https://doi.org/10.1016/j.ensm.2021.10.011. https://www.osti.gov/servlets/purl/1840534.
@article{osti_1840534,
title = {Methodologies for Design, Characterization and Testing of Electrolytes that Enable Extreme Fast Charging of Lithium-ion Cells},
author = {Gao, Ningshengjie and Kim, Sangwook and Chinnam, Parameswara and Dufek, Eric J. and Colclasure, Andrew M. and Jansen, Andrew and Son, Seoung-Bum and Bloom, Ira and Dunlop, Alison and Trask, Stephen and Gering, Kevin L.},
abstractNote = {Selection, testing and validation of electrolyte candidates for Li-ion cells are discussed, based on a 10-minute target for extreme fast charge (XFC). A combination of modeling and laboratory measurements create a timely and synergistic approach to identifying candidate electrolyte formulations. Multi-solvent systems provide a balanced set of properties, wherein lower molecular-weight solvents offer reduced viscosity, increased species diffusivity, and mitigation of concentration polarization at high charge rates. Carefully selected formulations can exhibit peak conductivity and usable conductivity range of two to three times that of the baseline EC-EMC (3:7, wt.) + LiPF6. Candidates are also chosen based on stability and longevity within the cell environment. Lab testing coincides with property predictions from the Advanced Electrolyte Model (AEM) and a macro-scale cell model. Furthermore, cell testing utilized coin and pouch cells having NMC532 or NMC811 cathodes with graphite electrodes. Results indicate combinations of low-molecular weight solvents are key for fast-charge electrolytes as they extend the useful conductivity range to both low and higher salt concentrations, and possess higher self-diffusivities compared to conventional solvents. This reduces impacts from concentration polarization. The choice of electrolyte also influences the tendency for lithium metal deposition at the anode, as showcased by experimental and modeling results herein.},
doi = {10.1016/j.ensm.2021.10.011},
journal = {Energy Storage Materials},
number = ,
volume = 44,
place = {United States},
year = {Sat Oct 09 00:00:00 EDT 2021},
month = {Sat Oct 09 00:00:00 EDT 2021}
}

Works referenced in this record:

A review of the features and analyses of the solid electrolyte interphase in Li-ion batteries
journal, September 2010


Fingerprinting Redox Heterogeneity in Electrodes during Extreme Fast Charging
journal, May 2020

  • Mistry, Aashutosh; Usseglio-Viretta, Francois L. E.; Colclasure, Andrew
  • Journal of The Electrochemical Society, Vol. 167, Issue 9
  • DOI: 10.1149/1945-7111/ab8fd7

Quantification of Inactive Lithium and Solid–Electrolyte Interphase Species on Graphite Electrodes after Fast Charging
journal, May 2020


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


A convective transport theory for high rate discharge in lithium ion cells
journal, January 2013


Investigating the solid electrolyte interphase using binder-free graphite electrodes
journal, January 2008


A Critical Evaluation of the Advanced Electrolyte Model
journal, January 2018

  • Logan, E. R.; Tonita, Erin M.; Gering, K. L.
  • Journal of The Electrochemical Society, Vol. 165, Issue 14
  • DOI: 10.1149/2.0471814jes

Effects of Electrolyte Composition on Lithium Plating in Lithium-Ion Cells
journal, January 2011

  • Smart, M. C.; Ratnakumar, B. V.
  • Journal of The Electrochemical Society, Vol. 158, Issue 4
  • DOI: 10.1149/1.3544439

Heterogeneous Behavior of Lithium Plating during Extreme Fast Charging
journal, July 2020


In Operando Detection of the Onset and Mapping of Lithium Plating Regimes during Fast Charging of Lithium-Ion Batteries
journal, June 2020

  • Fear, Conner; Adhikary, Tanay; Carter, Rachel
  • ACS Applied Materials & Interfaces, Vol. 12, Issue 27
  • DOI: 10.1021/acsami.0c07803

Investigation of Lithium Plating-Stripping Process in Li-Ion Batteries at Low Temperature Using an Electrochemical Model
journal, January 2018

  • Ren, Dongsheng; Smith, Kandler; Guo, Dongxu
  • Journal of The Electrochemical Society, Vol. 165, Issue 10
  • DOI: 10.1149/2.0661810jes

Effect of Capillary Element Aspect Ratio on the Dynamic Imbibition within Porous Networks
journal, August 2002

  • Ridgway, Cathy J.; Gane, Patrick A. C.; Schoelkopf, Joachim
  • Journal of Colloid and Interface Science, Vol. 252, Issue 2
  • DOI: 10.1006/jcis.2002.8468

Electrolyte Development for High-Performance Li-Ion Cells: Additives, Solvents, and Agreement with a Generalized Molecular Model
journal, January 2019

  • Logan, Eric R.; Gering, Kevin L.; Ma, Xiaowei
  • The Electrochemical Society Interface, Vol. 28, Issue 2
  • DOI: 10.1149/2.F04192if

Solute-volume effects in electrolyte transport
journal, July 2014


Lithium plating in lithium-ion batteries at sub-ambient temperatures investigated by in situ neutron diffraction
journal, December 2014


Requirements for Enabling Extreme Fast Charging of High Energy Density Li-Ion Cells while Avoiding Lithium Plating
journal, January 2019

  • Colclasure, Andrew M.; Dunlop, Alison R.; Trask, Stephen E.
  • Journal of The Electrochemical Society, Vol. 166, Issue 8
  • DOI: 10.1149/2.0451908jes

Fast Charging of Li-Ion Cells: Part IV. Temperature Effects and “Safe Lines” to Avoid Lithium Plating
journal, September 2020

  • Rodrigues, Marco-Tulio F.; Shkrob, Ilya A.; Colclasure, Andrew M.
  • Journal of The Electrochemical Society, Vol. 167, Issue 13
  • DOI: 10.1149/1945-7111/abb70d

In situ X-ray spatial profiling reveals uneven compression of electrode assemblies and steep lateral gradients in lithium-ion coin cells
journal, January 2020

  • Okasinski, John S.; Shkrob, Ilya A.; Chuang, Andrew
  • Physical Chemistry Chemical Physics, Vol. 22, Issue 38
  • DOI: 10.1039/D0CP04436A

Fast Charge-Driven Li Plating on Anode and Structural Degradation of Cathode
journal, October 2020

  • Son, Seoung-Bum; Robertson, David; Yang, Zhenzhen
  • Journal of The Electrochemical Society, Vol. 167, Issue 14
  • DOI: 10.1149/1945-7111/abc031

Quantitative and time-resolved detection of lithium plating on graphite anodes in lithium ion batteries
journal, April 2018


Spatial dynamics of lithiation and lithium plating during high-rate operation of graphite electrodes
journal, January 2020

  • Finegan, Donal P.; Quinn, Alexander; Wragg, David S.
  • Energy & Environmental Science, Vol. 13, Issue 8
  • DOI: 10.1039/D0EE01191F

Fast Charging of Lithium-ion Batteries via Electrode Engineering
journal, January 2020

  • Vishnugopi, Bairav S.; Verma, Ankit; Mukherjee, Partha P.
  • Journal of The Electrochemical Society, Vol. 167, Issue 9
  • DOI: 10.1149/1945-7111/ab7fb9

Enabling fast charging – Introduction and overview
journal, November 2017


Apparent Increasing Lithium Diffusion Coefficient with Applied Current in Graphite
journal, August 2020

  • Dees, Dennis W.; Rodrigues, Marco-Tulio F.; Kalaga, Kaushik
  • Journal of The Electrochemical Society, Vol. 167, Issue 12
  • DOI: 10.1149/1945-7111/abaf9f

Lithium-ion battery fast charging: A review
journal, August 2019


Low-temperature study of lithium-ion cells using a LiySn micro-reference electrode
journal, December 2007


Li plating as unwanted side reaction in commercial Li-ion cells – A review
journal, April 2018


Electrode scale and electrolyte transport effects on extreme fast charging of lithium-ion cells
journal, March 2020


Challenges and opportunities towards fast-charging battery materials
journal, June 2019


Anode potential controlled charging prevents lithium plating
journal, January 2020

  • Rangarajan, Sobana P.; Barsukov, Yevgen; Mukherjee, Partha P.
  • Journal of Materials Chemistry A, Vol. 8, Issue 26
  • DOI: 10.1039/D0TA04467A

How Fast Can a Li-Ion Battery Be Charged? Determination of Limiting Fast Charging Conditions
journal, January 2021

  • F. Rodrigues, Marco T.; Son, Seoung-Bum; Colclasure, Andrew M.
  • ACS Applied Energy Materials, Vol. 4, Issue 2
  • DOI: 10.1021/acsaem.0c03114

Exploring Classes of Co-Solvents for Fast-Charging Lithium-Ion Cells
journal, January 2018

  • Hall, David S.; Eldesoky, Ahmed; Logan, E. R.
  • Journal of The Electrochemical Society, Vol. 165, Issue 10
  • DOI: 10.1149/2.1351810jes

Analysis of internal short-circuit in a lithium ion cell
journal, October 2009

  • Santhanagopalan, Shriram; Ramadass, Premanand; Zhang, John (Zhengming)
  • Journal of Power Sources, Vol. 194, Issue 1, p. 550-557
  • DOI: 10.1016/j.jpowsour.2009.05.002

Extreme Fast Charge Challenges for Lithium-Ion Battery: Variability and Positive Electrode Issues
journal, January 2019

  • Tanim, Tanvir R.; Dufek, Eric J.; Evans, Michael
  • Journal of The Electrochemical Society, Vol. 166, Issue 10
  • DOI: 10.1149/2.0731910jes