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Title: Correlation of Electrolyte Volume and Electrochemical Performance in Lithium-Ion Pouch Cells with Graphite Anodes and NMC532 Cathodes

Abstract

The work herein reports on studies aimed at exploring the correlation between electrolyte volume and electrochemical performance of full cell, pouch-cells consisting of graphite/ Li 1.02Ni 0.50Mn 0.29Co 0.19O 2 (NMC-532) as the electrodes and 1.2 M LiPF 6 in ethylene carbonate:ethylmethyl carbonate (EC:EMC) as the electrolyte. In addition, it is demonstrated that a minimum electrolyte volume factor of 1.9 times the total pore volume of cell components (cathode, anode, and separator) is needed for long-term cyclability and low impedance. Less electrolyte results in an increase of the measured Ohmic resistances. Increased resistance ratios for charge transfer and passivation layers at cathode, relative to initial values, were 1.5 2.0 after 100 cycles. At the cathode, the resistance from charge transfer was 2-3 times higher than for passivation layers. Lastly, differential voltage analysis showed that anodes were less delithiated after discharging as the cells were cycled.

Authors:
 [1];  [1];  [2];  [1];  [3];  [3];  [3];  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Energy & Transportation Science Division; Univ. of Tennessee, Knoxville, TN (United States). Bredesen Center for Interdisciplinary Research and Graduate Education
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Energy & Transportation Science Division
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1352759
Grant/Contract Number:
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 164; Journal Issue: 6; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 25 ENERGY STORAGE; Electrolyte volume; cycle life; lithium ion battery; full pouch cell; high voltage; resistance

Citation Formats

An, Seong Jin, Li, Jianlin, Mohanty, Debasish, Daniel, Claus, Polzin, Bryant J., Croy, Jason R., E. Trask, Stephen, and Wood, David L. Correlation of Electrolyte Volume and Electrochemical Performance in Lithium-Ion Pouch Cells with Graphite Anodes and NMC532 Cathodes. United States: N. p., 2017. Web. doi:10.1149/2.1131706jes.
An, Seong Jin, Li, Jianlin, Mohanty, Debasish, Daniel, Claus, Polzin, Bryant J., Croy, Jason R., E. Trask, Stephen, & Wood, David L. Correlation of Electrolyte Volume and Electrochemical Performance in Lithium-Ion Pouch Cells with Graphite Anodes and NMC532 Cathodes. United States. doi:10.1149/2.1131706jes.
An, Seong Jin, Li, Jianlin, Mohanty, Debasish, Daniel, Claus, Polzin, Bryant J., Croy, Jason R., E. Trask, Stephen, and Wood, David L. Fri . "Correlation of Electrolyte Volume and Electrochemical Performance in Lithium-Ion Pouch Cells with Graphite Anodes and NMC532 Cathodes". United States. doi:10.1149/2.1131706jes. https://www.osti.gov/servlets/purl/1352759.
@article{osti_1352759,
title = {Correlation of Electrolyte Volume and Electrochemical Performance in Lithium-Ion Pouch Cells with Graphite Anodes and NMC532 Cathodes},
author = {An, Seong Jin and Li, Jianlin and Mohanty, Debasish and Daniel, Claus and Polzin, Bryant J. and Croy, Jason R. and E. Trask, Stephen and Wood, David L.},
abstractNote = {The work herein reports on studies aimed at exploring the correlation between electrolyte volume and electrochemical performance of full cell, pouch-cells consisting of graphite/ Li1.02Ni0.50Mn0.29Co0.19O2 (NMC-532) as the electrodes and 1.2 M LiPF6 in ethylene carbonate:ethylmethyl carbonate (EC:EMC) as the electrolyte. In addition, it is demonstrated that a minimum electrolyte volume factor of 1.9 times the total pore volume of cell components (cathode, anode, and separator) is needed for long-term cyclability and low impedance. Less electrolyte results in an increase of the measured Ohmic resistances. Increased resistance ratios for charge transfer and passivation layers at cathode, relative to initial values, were 1.5 2.0 after 100 cycles. At the cathode, the resistance from charge transfer was 2-3 times higher than for passivation layers. Lastly, differential voltage analysis showed that anodes were less delithiated after discharging as the cells were cycled.},
doi = {10.1149/2.1131706jes},
journal = {Journal of the Electrochemical Society},
number = 6,
volume = 164,
place = {United States},
year = {Fri Apr 07 00:00:00 EDT 2017},
month = {Fri Apr 07 00:00:00 EDT 2017}
}

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Cited by: 3works
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  • The work herein reports on studies aimed at exploring the correlation between electrolyte volume and electrochemical performance of full cell, pouch-cells consisting of graphite/ Li 1.02Ni 0.50Mn 0.29Co 0.19O 2 (NMC-532) as the electrodes and 1.2 M LiPF6 in ethylene carbonate:ethylmethyl carbonate (EC:EMC) as the electrolyte. It is demonstrated that a minimum electrolyte volume factor of 1.9 times the total pore volume of cell components (cathode, anode, and separator) is needed for long-term cyclability and low impedance. Less electrolyte results in an increase of the measured ohmic resistances. Increased resistance ratios for charge transfer and passivation layers at cathode, relativemore » to initial values, were 1.5–2.0 after 100 cycles. At the cathode, the resistance from charge transfer was 2–3 times higher than for passivation layers. Differential voltage analysis showed that anodes were less delithiated after discharging as the cells were cycled.« less
  • This study aims to explore the correlations between electrolyte volume, electrochemical performance, and properties of the solid electrolyte interphase in pouch cells with Si-graphite composite anodes. The electrolyte is 1.2 M LiPF 6 in ethylene carbonate:ethylmethyl carbonate with 10 wt.% fluoroethylene carbonate. Single layer pouch cells (100 mAh) were constructed with 15 wt.% Si-graphite/LiNi 0.5Mn 0.3CO 0.2O 2 electrodes. It is found that a minimum electrolyte volume factor of 3.1 times the total pore volume of cell components (cathode, anode, and separator) is needed for better cycling stability. Less electrolyte causes increases in ohmic and charge transfer resistances. Lithium dendritesmore » are observed when the electrolyte volume factor is low. The resistances from the anodes become significant as the cells are discharged. As a result, solid electrolyte interphase thickness grows as the electrolyte volume factor increases and is non-uniform after cycling.« less
  • This study aims to explore the correlations between electrolyte volume, electrochemical performance, and properties of the solid electrolyte interphase in pouch cells with Si-graphite composite anodes. The electrolyte is 1.2 M LiPF 6 in ethylene carbonate:ethylmethyl carbonate with 10 wt % fluoroethylene carbonate. Single layer pouch cells (100 mA h) were constructed with 15 wt % Si-graphite/LiNi 0.5Mn 0.3CO 0.2O 2 electrodes. It is found that a minimum electrolyte volume factor of 3.1 times to the total pore volume of cell components (cathode, anode, and separator) is needed for better cycling stability. Less electrolyte causes increases in ohmic and chargemore » transfer resistances. Lithium dendrites are observed when the electrolyte volume factor is low. As a result, the resistances from the anodes become significant as the cells are discharged. Solid electrolyte interphase thickness grows as the electrolyte volume factor increases and is nonuniform after cycling.« less
  • In this article we describe efforts to improve performance and cycle life of cells containing Li1.2Ni0.15Mn0.55Co0.1O2-based positive and graphite-based negative electrodes. Initial work to identify high-performing materials, compositions, fabrication variables, and cycling conditions is conducted in coin cells. The resulting information is then used for the preparation of double-sided electrodes, assembly of pouch cells, and electrochemical testing. We report the cycling performance of cells with electrodes prepared under various conditions. Our data indicate that cells with positive electrodes containing 92 wt% Li1.2Ni0.15Mn0.55Co0.1O2, 4 wt% carbons (no graphite), and 4 wt% PVdF (92-4-4) show ~20% capacity fade after 1000 cycles inmore » the 2.5-4.4V range, significantly better than our baseline cells that show the same fade after only 450 cycles. Our analyses indicate that the major contributors to cell energy fade are capacity loss and impedance rise. Therefore incorporating approaches that minimize capacity fade and impedance rise, such as electrode coatings and electrolyte additives, can significantly enhance calendar and cycle life of this promising cell chemistry.« less
  • Lithium-ion batteries have started replacing the conventional aqueous nickel-based battery systems in space applications, such as planetary landers, rovers, orbiters and satellites. The reasons for such widespread use of these batteries are the savings in mass and volume of the power subsystems, resulting from their high gravimetric and volumetric energy densities, and their ability to operate at extreme temperatures. In our pursuit to further enhance the specific energy as well as low-temperature performance of Li-ion batteries, we have been investigating various layered lithiated metal oxides, e.g., LiCoO{sub 2}, LiNi{sub 0.8}Co{sub 0.2} and LiNi{sub 0.8}Co{sub 0.15}Al{sub 0.05}O{sub 2}, as well asmore » different low-temperature electrolytes, including ternary and quaternary carbonate mixtures with various co-solvents. In this paper, we report our recent studies on Li{sub 1+x}(Co{sub 1/3}Ni{sub 1/3}Mn{sub 1/3}){sub 1-x}O{sub 2} cathodes, combined with three different low-temperature electrolytes, i.e.: (1) 1.0 M LiPF{sub 6} in EC:EMC (20:80), (2) 1.2 M LiPF{sub 6} in EC:EMC (20:80) and (3) 1.2 M LiPF{sub 6} in EC:EMC (30:70). Electrical performance characteristics were determined in laboratory glass cells at different discharge rates and different temperatures. Further, individual electrode kinetics of both Li{sub 1+x}(Co{sub 1/3}Ni{sub 1/3}Mn{sub 1/3}){sub 1-x}O{sub 2} cathodes and MCMB graphite anodes were determined at different temperatures, using dc micropolarization, Tafel polarization and electrochemical impedance spectroscopy (EIS). Analysis of these data has led to interesting trends relative to the effects of solvent composition and salt concentration, on the electrical performance and on the kinetics of cathode and anode.« less