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

Abstract

Increasing the charge rate of Li-ion cells over 1–2C (full charge in 30–60 min) would be highly desirable, but high currents flowing through the active materials push these cells to their endurance limits. In this article, we aim to understand how such high-current regimes affect electrochemical properties of the cells. Formation of Li metal deposits is a recognized hazard of high-rate charging, as Li plating can overtake lithium intercalation in the negative electrode. Here we demonstrate how microprobe Li/Cu reference electrodes can be used to characterize the graphite anode and layered oxide (NCM523) cathode during constant-current (≤ 6C) voltage-limited (4.39 V) charging of Li-ion cells. These reference electrodes are used to monitor the onset of Li plating conditions in situ during cell charging. As the current increases over 3C, the anode potentials decrease below -40 mV causing lithium nucleation. Surprisingly, this nucleation (at least, initially) does not result in capacity fade or a higher anode impedance even in strongly polarized cells, so it appears that the nascent Li nuclei are isolated from electrolyte by the pre-existing solid electrolyte interphase. Our study shows that microprobe reference electrodes are an important diagnostic tool to characterize full-cell behavior in the high-current regimes.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
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:
1505137
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 166; Journal Issue: 6; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; batteries - lithium; energy storage; fast charge; graphite anode; lithium plating

Citation Formats

Rodrigues, Marco-Tulio F., Kalaga, Kaushik, Trask, Stephen E., Dees, Dennis W., Shkrob, Ilya A., and Abraham, Daniel P. Fast Charging of Li-Ion Cells: Part I. Using Li/Cu Reference Electrodes to Probe Individual Electrode Potentials. United States: N. p., 2019. Web. doi:10.1149/2.0401906jes.
Rodrigues, Marco-Tulio F., Kalaga, Kaushik, Trask, Stephen E., Dees, Dennis W., Shkrob, Ilya A., & Abraham, Daniel P. Fast Charging of Li-Ion Cells: Part I. Using Li/Cu Reference Electrodes to Probe Individual Electrode Potentials. United States. doi:10.1149/2.0401906jes.
Rodrigues, Marco-Tulio F., Kalaga, Kaushik, Trask, Stephen E., Dees, Dennis W., Shkrob, Ilya A., and Abraham, Daniel P. Wed . "Fast Charging of Li-Ion Cells: Part I. Using Li/Cu Reference Electrodes to Probe Individual Electrode Potentials". United States. doi:10.1149/2.0401906jes. https://www.osti.gov/servlets/purl/1505137.
@article{osti_1505137,
title = {Fast Charging of Li-Ion Cells: Part I. Using Li/Cu Reference Electrodes to Probe Individual Electrode Potentials},
author = {Rodrigues, Marco-Tulio F. and Kalaga, Kaushik and Trask, Stephen E. and Dees, Dennis W. and Shkrob, Ilya A. and Abraham, Daniel P.},
abstractNote = {Increasing the charge rate of Li-ion cells over 1–2C (full charge in 30–60 min) would be highly desirable, but high currents flowing through the active materials push these cells to their endurance limits. In this article, we aim to understand how such high-current regimes affect electrochemical properties of the cells. Formation of Li metal deposits is a recognized hazard of high-rate charging, as Li plating can overtake lithium intercalation in the negative electrode. Here we demonstrate how microprobe Li/Cu reference electrodes can be used to characterize the graphite anode and layered oxide (NCM523) cathode during constant-current (≤ 6C) voltage-limited (4.39 V) charging of Li-ion cells. These reference electrodes are used to monitor the onset of Li plating conditions in situ during cell charging. As the current increases over 3C, the anode potentials decrease below -40 mV causing lithium nucleation. Surprisingly, this nucleation (at least, initially) does not result in capacity fade or a higher anode impedance even in strongly polarized cells, so it appears that the nascent Li nuclei are isolated from electrolyte by the pre-existing solid electrolyte interphase. Our study shows that microprobe reference electrodes are an important diagnostic tool to characterize full-cell behavior in the high-current regimes.},
doi = {10.1149/2.0401906jes},
journal = {Journal of the Electrochemical Society},
number = 6,
volume = 166,
place = {United States},
year = {2019},
month = {3}
}

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