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Title: Calendar-life versus cycle-life aging of lithium-ion cells with silicon-graphite composite electrodes

Abstract

The use of blended silicon-graphite (Si-Gr) negative electrodes increases the energy density of lithium-ion cells over those containing only graphite (Gr) electrodes. However, volume changes in the Si particles that occur during cycling causes deterioration of the solid-electrolyte interphase (SEI) layer on the particles resulting in further electrolyte reduction that immobilizes Li+ ions and, therefore, capacity fade. Because the volume changes are not expected to occur during a potentiostatic hold (referred to as calendar-life aging), by comparison of cycle-life and calendar-life aged cells one can expect to assess the role of volume changes in the deterioration of cell performance. To this end, cells with Si-Gr and Gr negative electrodes (and Li1.03(Ni0.5Co0.2Mn0.3)0.97O2 containing positive electrodes) were assembled, tested, and compared using cycle-life and calendar-life aging protocols. As expected, the capacity loss of the cycle-life aged cells was higher than that of the calendar-life aged cells. However, the measurable capacity loss for the calendar-life aged cells indicated continued immobilization of Li+ ions. Furthermore, electrolytes extracted from the calendar-life aged cells showed more LiPF6 hydrolysis products than those extracted from the cycle-life aged cells. In conclusion, we discuss possible mechanistic causes for the observed aging behaviors in this article.

Authors:
 [1];  [1];  [1];  [1];  [1]
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  1. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)
OSTI Identifier:
1465507
Alternate Identifier(s):
OSTI ID: 1562991
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Electrochimica Acta
Additional Journal Information:
Journal Volume: 280; Journal Issue: C; Journal ID: ISSN 0013-4686
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; FEC; NCM523; electrochemical performance; electrolyte NMR; reference electrode

Citation Formats

Kalaga, Kaushik, Rodrigues, Marco-Tulio F., Trask, Stephen E., Shkrob, Ilya A., and Abraham, Daniel P. Calendar-life versus cycle-life aging of lithium-ion cells with silicon-graphite composite electrodes. United States: N. p., 2018. Web. doi:10.1016/j.electacta.2018.05.101.
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Kalaga, Kaushik, Rodrigues, Marco-Tulio F., Trask, Stephen E., Shkrob, Ilya A., & Abraham, Daniel P. Calendar-life versus cycle-life aging of lithium-ion cells with silicon-graphite composite electrodes. United States. https://doi.org/10.1016/j.electacta.2018.05.101
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Kalaga, Kaushik, Rodrigues, Marco-Tulio F., Trask, Stephen E., Shkrob, Ilya A., and Abraham, Daniel P. Thu . "Calendar-life versus cycle-life aging of lithium-ion cells with silicon-graphite composite electrodes". United States. https://doi.org/10.1016/j.electacta.2018.05.101. https://www.osti.gov/servlets/purl/1465507.
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@article{osti_1465507,
title = {Calendar-life versus cycle-life aging of lithium-ion cells with silicon-graphite composite electrodes},
author = {Kalaga, Kaushik and Rodrigues, Marco-Tulio F. and Trask, Stephen E. and Shkrob, Ilya A. and Abraham, Daniel P.},
abstractNote = {The use of blended silicon-graphite (Si-Gr) negative electrodes increases the energy density of lithium-ion cells over those containing only graphite (Gr) electrodes. However, volume changes in the Si particles that occur during cycling causes deterioration of the solid-electrolyte interphase (SEI) layer on the particles resulting in further electrolyte reduction that immobilizes Li+ ions and, therefore, capacity fade. Because the volume changes are not expected to occur during a potentiostatic hold (referred to as calendar-life aging), by comparison of cycle-life and calendar-life aged cells one can expect to assess the role of volume changes in the deterioration of cell performance. To this end, cells with Si-Gr and Gr negative electrodes (and Li1.03(Ni0.5Co0.2Mn0.3)0.97O2 containing positive electrodes) were assembled, tested, and compared using cycle-life and calendar-life aging protocols. As expected, the capacity loss of the cycle-life aged cells was higher than that of the calendar-life aged cells. However, the measurable capacity loss for the calendar-life aged cells indicated continued immobilization of Li+ ions. Furthermore, electrolytes extracted from the calendar-life aged cells showed more LiPF6 hydrolysis products than those extracted from the cycle-life aged cells. In conclusion, we discuss possible mechanistic causes for the observed aging behaviors in this article.},
doi = {10.1016/j.electacta.2018.05.101},
journal = {Electrochimica Acta},
number = C,
volume = 280,
place = {United States},
year = {Thu May 17 00:00:00 EDT 2018},
month = {Thu May 17 00:00:00 EDT 2018}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1016/j.electacta.2018.05.101
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Cited by: 61 works
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Figures / Tables:

Table 1 Table 1: Capacity values (mAh goxide-1) during calendar-life testing of a NCM523/Si-Gr cell (FEC electrolyte).
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    Works referencing / citing this record:

    Fast Charging of Li-Ion Cells: Part I. Using Li/Cu Reference Electrodes to Probe Individual Electrode Potentials
    journal, January 2019

    • Rodrigues, Marco-Tulio F.; Kalaga, Kaushik; Trask, Stephen E.
    • Journal of The Electrochemical Society, Vol. 166, Issue 6
    • DOI: 10.1149/2.0401906jes

    Critical Review of the Use of Reference Electrodes in Li-Ion Batteries: A Diagnostic Perspective
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    Rapid coating of asphalt to prepare carbon-encapsulated composites of nano-silicon and graphite for lithium battery anodes
    journal, December 2019

    Operando Quantification of (De)Lithiation Behavior of Silicon-Graphite Blended Electrodes for Lithium-Ion Batteries
    journal, January 2019

    • Yao, Koffi P. C.; Okasinski, John S.; Kalaga, Kaushik
    • Advanced Energy Materials, Vol. 9, Issue 8
    • DOI: 10.1002/aenm.201803380
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      Figures / Tables found in this record:

      Table 1 (p. 19)table
      Table 2 (p. 20)table
      Table 3 (p. 21)table
      Fig. 1 (p. 22)figure
      Fig. 2 (p. 23)figure
      Fig. 3 (p. 24)figure
      Fig. 4 (p. 25)figure
      Fig. 5 (p. 26)figure
      Fig. 6 (p. 27)figure
      Fig. 7 (p. 28)figure
      Table S1 (p. 30)table
      Fig. S1 (p. 31)figure
      Fig. S2 (p. 32)figure
      Figure S3 (p. 33)figure
      Figure S4 (p. 34)figure
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