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Title: Electrolyte volume effects on electrochemical performance and solid electrolyte interphase in Si-graphite/NMC lithium-ion pouch cells

Abstract

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 dendrites 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.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1];  [2];  [3];  [3];  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Argonne National Lab. (ANL), Lemont, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States); 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:
1372400
Alternate Identifier(s):
OSTI ID: 1376392
Grant/Contract Number:
AC02-06CH11357; AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 9; Journal Issue: 22; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 25 ENERGY STORAGE; electrolyte volume; cycle life; lithium-ion; resistance; silicon-graphite anode; solid electrolyte interphase; lithium ion

Citation Formats

An, Seong Jin, Li, Jianlin, Daniel, Claus, Meyer, III, Harry M., Trask, Stephen E., Polzin, Bryant J., and Wood, David L.. Electrolyte volume effects on electrochemical performance and solid electrolyte interphase in Si-graphite/NMC lithium-ion pouch cells. United States: N. p., 2017. Web. doi:10.1021/acsami.7b03617.
An, Seong Jin, Li, Jianlin, Daniel, Claus, Meyer, III, Harry M., Trask, Stephen E., Polzin, Bryant J., & Wood, David L.. Electrolyte volume effects on electrochemical performance and solid electrolyte interphase in Si-graphite/NMC lithium-ion pouch cells. United States. doi:10.1021/acsami.7b03617.
An, Seong Jin, Li, Jianlin, Daniel, Claus, Meyer, III, Harry M., Trask, Stephen E., Polzin, Bryant J., and Wood, David L.. Mon . "Electrolyte volume effects on electrochemical performance and solid electrolyte interphase in Si-graphite/NMC lithium-ion pouch cells". United States. doi:10.1021/acsami.7b03617. https://www.osti.gov/servlets/purl/1372400.
@article{osti_1372400,
title = {Electrolyte volume effects on electrochemical performance and solid electrolyte interphase in Si-graphite/NMC lithium-ion pouch cells},
author = {An, Seong Jin and Li, Jianlin and Daniel, Claus and Meyer, III, Harry M. and Trask, Stephen E. and Polzin, Bryant J. and Wood, David L.},
abstractNote = {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 LiPF6 in ethylene carbonate:ethylmethyl carbonate with 10 wt.% fluoroethylene carbonate. Single layer pouch cells (100 mAh) were constructed with 15 wt.% Si-graphite/LiNi0.5Mn0.3CO0.2O2 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 dendrites 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.},
doi = {10.1021/acsami.7b03617},
journal = {ACS Applied Materials and Interfaces},
number = 22,
volume = 9,
place = {United States},
year = {Mon May 15 00:00:00 EDT 2017},
month = {Mon May 15 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
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Citation Metrics:
Cited by: 5works
Citation information provided by
Web of Science

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  • 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
  • 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
  • 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 layersmore » 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.« less
  • An in-depth review is presented on the science of lithium-ion battery (LIB) solid electrolyte interphase (SEI) formation on the graphite anode, including structure, morphology, chemical composition, electrochemistry, formation mechanism, and LIB formation cycling. During initial operation of LIBs, the SEI layer forms on the graphite surfaces, the most commonly used anode material, due to side reactions with the electrolyte solvent/salt at low electro-reduction potentials. It is accepted that the SEI layer is essential to the long-term performance of LIBs, and it also has an impact on its initial capacity loss, self-discharge characteristics, cycle life, rate capability, and safety. While themore » presence of the anode SEI layer is vital, it is difficult to control its formation and growth, as the chemical composition, morphology, and stability depend on several factors. These factors include the type of graphite, electrolyte composition, electrochemical conditions, and cell temperature. Thus, SEI layer formation and electrochemical stability over long-term operation should be a primary topic of future investigation in the development of LIB technology. We review the progression of knowledge gained about the anode SEI, from its discovery in 1979 to the current state of understanding, and covers its formation process, differences in the chemical and structural makeup when cell materials and components are varied, methods of characterization, and associated reactions with the liquid electrolyte phase. It also discusses the relationship of the SEI layer to the LIB formation step, which involves both electrolyte wetting and subsequent slow charge-discharge cycles to grow the SEI.« less
    Cited by 80
  • An in-depth review is presented on the science of lithium-ion battery (LIB) solid electrolyte interphase (SEI) formation on the graphite anode, including structure, morphology, chemical composition, electrochemistry, formation mechanism, and LIB formation cycling. During initial operation of LIBs, the SEI layer forms on the graphite surfaces, the most commonly used anode material, due to side reactions with the electrolyte solvent/salt at low electro-reduction potentials. It is accepted that the SEI layer is essential to the long-term performance of LIBs, and it also has an impact on its initial capacity loss, self-discharge characteristics, cycle life, rate capability, and safety. While themore » presence of the anode SEI layer is vital, it is difficult to control its formation and growth, as the chemical composition, morphology, and stability depend on several factors. These factors include the type of graphite, electrolyte composition, electrochemical conditions, and cell temperature. Thus, SEI layer formation and electrochemical stability over long-term operation should be a primary topic of future investigation in the development of LIB technology. We review the progression of knowledge gained about the anode SEI, from its discovery in 1979 to the current state of understanding, and covers its formation process, differences in the chemical and structural makeup when cell materials and components are varied, methods of characterization, and associated reactions with the liquid electrolyte phase. It also discusses the relationship of the SEI layer to the LIB formation step, which involves both electrolyte wetting and subsequent slow charge-discharge cycles to grow the SEI.« less