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Title: Selecting the Best Graphite for Long-Life, High-Energy Li-Ion Batteries

Here, most lithium-ion batteries still rely on intercalation-type graphite materials for anodes, so it is important to consider their role in full cells for applications in electric vehicles. Here, we systematically evaluate the chemical and physical properties of six commercially-available natural and synthetic graphites to establish which factors have the greatest impact on the cycling stability of full cells with nickel-rich LiNi0.8Mn0.1Co0.1O2 (NMC811) cathodes. Electrochemical data and post-mortem characterization explain the origin of capacity fade. The NMC811 cathode shows large irreversible capacity loss and impedance growth, accounting for much of full cell degradation. However, six graphite anodes demonstrate significant differences with respect to structural change, surface area, impedance growth, and SEI chemistry, which impact overall capacity retention. We found long cycle life correlated most strongly with stable graphite crystallite size. In addition, graphites with lower surface area generally had higher coulombic efficiencies during formation cycles, which led to more stable long-term cycling. The best graphite screened here enables a capacity retention around 90% in full pouch cells over extensive long-term cycling compared to only 82% for cells with the lowest performing graphite. The results show that optimal graphite selection improves cycling stability of high energy lithium-ion cells.
Authors:
ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1] ;  [2] ; ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [2]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 165; Journal Issue: 9; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; cycling stability; graphite anode; Ni-rich cathode
OSTI Identifier:
1456808

Mao, Chengyu, Wood, Marissa, David, Lamuel Abraham, An, Seong Jin, Sheng, Yangping, Du, Zhijia, Meyer, III, Harry M., Ruther, Rose E., and Wood, III, David L.. Selecting the Best Graphite for Long-Life, High-Energy Li-Ion Batteries. United States: N. p., Web. doi:10.1149/2.1111809jes.
Mao, Chengyu, Wood, Marissa, David, Lamuel Abraham, An, Seong Jin, Sheng, Yangping, Du, Zhijia, Meyer, III, Harry M., Ruther, Rose E., & Wood, III, David L.. Selecting the Best Graphite for Long-Life, High-Energy Li-Ion Batteries. United States. doi:10.1149/2.1111809jes.
Mao, Chengyu, Wood, Marissa, David, Lamuel Abraham, An, Seong Jin, Sheng, Yangping, Du, Zhijia, Meyer, III, Harry M., Ruther, Rose E., and Wood, III, David L.. 2018. "Selecting the Best Graphite for Long-Life, High-Energy Li-Ion Batteries". United States. doi:10.1149/2.1111809jes. https://www.osti.gov/servlets/purl/1456808.
@article{osti_1456808,
title = {Selecting the Best Graphite for Long-Life, High-Energy Li-Ion Batteries},
author = {Mao, Chengyu and Wood, Marissa and David, Lamuel Abraham and An, Seong Jin and Sheng, Yangping and Du, Zhijia and Meyer, III, Harry M. and Ruther, Rose E. and Wood, III, David L.},
abstractNote = {Here, most lithium-ion batteries still rely on intercalation-type graphite materials for anodes, so it is important to consider their role in full cells for applications in electric vehicles. Here, we systematically evaluate the chemical and physical properties of six commercially-available natural and synthetic graphites to establish which factors have the greatest impact on the cycling stability of full cells with nickel-rich LiNi0.8Mn0.1Co0.1O2 (NMC811) cathodes. Electrochemical data and post-mortem characterization explain the origin of capacity fade. The NMC811 cathode shows large irreversible capacity loss and impedance growth, accounting for much of full cell degradation. However, six graphite anodes demonstrate significant differences with respect to structural change, surface area, impedance growth, and SEI chemistry, which impact overall capacity retention. We found long cycle life correlated most strongly with stable graphite crystallite size. In addition, graphites with lower surface area generally had higher coulombic efficiencies during formation cycles, which led to more stable long-term cycling. The best graphite screened here enables a capacity retention around 90% in full pouch cells over extensive long-term cycling compared to only 82% for cells with the lowest performing graphite. The results show that optimal graphite selection improves cycling stability of high energy lithium-ion cells.},
doi = {10.1149/2.1111809jes},
journal = {Journal of the Electrochemical Society},
number = 9,
volume = 165,
place = {United States},
year = {2018},
month = {6}
}

Works referenced in this record:

Significant Improvement of Electrochemical Performance of AlF3-Coated Li[Ni0.8Co0.1Mn0.1]O2 Cathode Materials
journal, January 2007
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Lithium Ion Battery Graphite Solid Electrolyte Interphase Revealed by Microscopy and Spectroscopy
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