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Title: Transition metal dissolution, ion migration, electrocatalytic reduction and capacity loss in Lithium-ion full cells

Abstract

Continuous operation of full cells with layered transition metal (TM) oxide positive electrodes (NCM523) leads to dissolution of TM ions and their migration and incorporation into the solid electrolyte interphase (SEI) of the graphite-based negative electrode. These processes correlate with cell capacity fade and accelerate markedly as the upper cutoff voltage (UCV) exceeds 4.30 V. At voltages ≥ 4.4 V there is enhanced fracture of the oxide during cycling that creates new surfaces and causes increased solvent oxidation and TM dissolution. Despite this deterioration, cell capacity fade still mainly results from lithium loss in the negative electrode SEI. Among TMs, Mn content in the SEI shows a better correlation with cell capacity loss than Co and Ni contents. As Mn ions become incorporated into the SEI, the kinetics of lithium trapping change from power to linear at the higher UCVs, indicating a large effect of these ions on SEI growth and implicating (electro)catalytic reactions. Lastly, we estimate that each MnII ion deposited in the SEI causes trapping of ~102 additional Li+ ions thereby hastening the depletion of cyclable lithium ions. Using these results, we sketch a mechanism for cell capacity fade, emphasizing the conceptual picture over the chemical detail.

Authors:
 [1];  [1];  [1]
  1. Argonne National Lab. (ANL), Argonne, 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), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1339642
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 164; Journal Issue: 2; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; NCA; NCM523 oxide; SEI; electrochemistry; graphite; high voltage; layered oxides; manganese; nickel

Citation Formats

Gilbert, James A., Shkrob, Ilya A., and Abraham, Daniel P. Transition metal dissolution, ion migration, electrocatalytic reduction and capacity loss in Lithium-ion full cells. United States: N. p., 2017. Web. https://doi.org/10.1149/2.1111702jes.
Gilbert, James A., Shkrob, Ilya A., & Abraham, Daniel P. Transition metal dissolution, ion migration, electrocatalytic reduction and capacity loss in Lithium-ion full cells. United States. https://doi.org/10.1149/2.1111702jes
Gilbert, James A., Shkrob, Ilya A., and Abraham, Daniel P. Thu . "Transition metal dissolution, ion migration, electrocatalytic reduction and capacity loss in Lithium-ion full cells". United States. https://doi.org/10.1149/2.1111702jes. https://www.osti.gov/servlets/purl/1339642.
@article{osti_1339642,
title = {Transition metal dissolution, ion migration, electrocatalytic reduction and capacity loss in Lithium-ion full cells},
author = {Gilbert, James A. and Shkrob, Ilya A. and Abraham, Daniel P.},
abstractNote = {Continuous operation of full cells with layered transition metal (TM) oxide positive electrodes (NCM523) leads to dissolution of TM ions and their migration and incorporation into the solid electrolyte interphase (SEI) of the graphite-based negative electrode. These processes correlate with cell capacity fade and accelerate markedly as the upper cutoff voltage (UCV) exceeds 4.30 V. At voltages ≥ 4.4 V there is enhanced fracture of the oxide during cycling that creates new surfaces and causes increased solvent oxidation and TM dissolution. Despite this deterioration, cell capacity fade still mainly results from lithium loss in the negative electrode SEI. Among TMs, Mn content in the SEI shows a better correlation with cell capacity loss than Co and Ni contents. As Mn ions become incorporated into the SEI, the kinetics of lithium trapping change from power to linear at the higher UCVs, indicating a large effect of these ions on SEI growth and implicating (electro)catalytic reactions. Lastly, we estimate that each MnII ion deposited in the SEI causes trapping of ~102 additional Li+ ions thereby hastening the depletion of cyclable lithium ions. Using these results, we sketch a mechanism for cell capacity fade, emphasizing the conceptual picture over the chemical detail.},
doi = {10.1149/2.1111702jes},
journal = {Journal of the Electrochemical Society},
number = 2,
volume = 164,
place = {United States},
year = {2017},
month = {1}
}

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    • DOI: 10.1149/2.0491811jes

    Electrolyte and SEI Decomposition Reactions of Transition Metal Ions Investigated by On-Line Electrochemical Mass Spectrometry
    journal, January 2018

    • Solchenbach, Sophie; Hong, Gloria; Freiberg, Anna Teresa Sophie
    • Journal of The Electrochemical Society, Vol. 165, Issue 14
    • DOI: 10.1149/2.0511814jes

    Review—Multifunctional Separators: A Promising Approach for Improving the Durability and Performance of Li-Ion Batteries
    journal, January 2019

    • Banerjee, Anjan; Ziv, Baruch; Shilina, Yuliya
    • Journal of The Electrochemical Society, Vol. 166, Issue 3
    • DOI: 10.1149/2.0561903jes

    Comparative Measurements of Side-Reaction Currents of Li[Li 1/3 Ti 5/3 ]O 4 and Li[Li 0.1 Al 0.1 Mn 1.8 ]O 4 Electrodes in Lithium-Ion Cells and Symmetric Cells
    journal, January 2019

    • Ariyoshi, Kingo; Fukunishi, Yuki; Yamada, Yusuke
    • Journal of The Electrochemical Society, Vol. 166, Issue 14
    • DOI: 10.1149/2.0601914jes

    Preformed Anodes for High-Voltage Lithium-Ion Battery Performance: Fluorinated Electrolytes, Crosstalk, and the Origins of Impedance Rise
    journal, January 2018

    • Tornheim, Adam; Sahore, Ritu; He, Meinan
    • Journal of The Electrochemical Society, Vol. 165, Issue 14
    • DOI: 10.1149/2.0611814jes

    One Law to Rule Them All: Stretched Exponential Master Curve of Capacity Fade for Li-Ion Batteries
    journal, January 2019

    • Cuervo-Reyes, Eduardo; Flückiger, Reto
    • Journal of The Electrochemical Society, Vol. 166, Issue 8
    • DOI: 10.1149/2.0611908jes

    Quantifying Changes to the Electrolyte and Negative Electrode in Aged NMC532/Graphite Lithium-Ion Cells
    journal, January 2018

    • Thompson, L. M.; Stone, W.; Eldesoky, A.
    • Journal of The Electrochemical Society, Vol. 165, Issue 11
    • DOI: 10.1149/2.0721811jes

    Effect of Choices of Positive Electrode Material, Electrolyte, Upper Cut-Off Voltage and Testing Temperature on the Life Time of Lithium-Ion Cells
    journal, January 2018

    • Li, Jing; Glazier, Stephen L.; Nelson, Kathlyne
    • Journal of The Electrochemical Society, Vol. 165, Issue 13
    • DOI: 10.1149/2.0931813jes

    Development of Electrolytes for Single Crystal NMC532/Artificial Graphite Cells with Long Lifetime
    journal, January 2018

    • Li, Jing; Li, Hongyang; Stone, Will
    • Journal of The Electrochemical Society, Vol. 165, Issue 3
    • DOI: 10.1149/2.0971803jes

    Nickel, Manganese, and Cobalt Dissolution from Ni-Rich NMC and Their Effects on NMC622-Graphite Cells
    journal, January 2019

    • Jung, Roland; Linsenmann, Fabian; Thomas, Rowena
    • Journal of The Electrochemical Society, Vol. 166, Issue 2
    • DOI: 10.1149/2.1151902jes

    A Guide to Full Coin Cell Making for Academic Researchers
    journal, January 2019

    • Murray, Vivian; Hall, David S.; Dahn, J. R.
    • Journal of The Electrochemical Society, Vol. 166, Issue 2
    • DOI: 10.1149/2.1171902jes

    Advancing Lithium- and Manganese-Rich Cathodes through a Combined Electrolyte Additive/Surface Treatment Strategy
    journal, January 2019

    • Gutierrez, Arturo; He, Meinan; Yonemoto, Bryan T.
    • Journal of The Electrochemical Society, Vol. 166, Issue 16
    • DOI: 10.1149/2.1281915jes

    Degradation and Aging Routes of Ni-Rich Cathode Based Li-Ion Batteries
    journal, January 2020

    • Teichert, Philipp; Eshetu, Gebrekidan Gebresilassie; Jahnke, Hannes
    • Batteries, Vol. 6, Issue 1
    • DOI: 10.3390/batteries6010008