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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 Li 1.03(Ni 0.5Co 0.2Mn 0.3) 0.97O 2 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 LiPF 6 hydrolysis products than those extracted from the cycle-life aged cells. In conclusion, we discuss possible mechanistic causes for the observed agingmore » behaviors in this article.« less

Authors:
 [1];  [1];  [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:
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.
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. doi:10.1016/j.electacta.2018.05.101.
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. doi:10.1016/j.electacta.2018.05.101. https://www.osti.gov/servlets/purl/1465507.
@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 = {2018},
month = {5}
}

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