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

doi:10.1149/2.1111809jes

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:

; ; ; An, Seong Jin ^[2] ; ; ; ; ;

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

Publication Date:: 2018-06-16

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.

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                    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.

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                    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.

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@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}

}

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Free Publicly Accessible Full Text
Accepted Manuscript (DOE)
Publisher's Version of Record
10.1149/2.1111809jes
https://doi.org/10.1149/2.1111809jes

Works referenced in this record:

Significant Improvement of Electrochemical Performance of AlF₃-Coated Li[Ni_0.8Co_0.1Mn_0.1]O₂ Cathode Materials
journal, January 2007

Woo, S.-U.; Yoon, C. S.; Amine, K.
Journal of The Electrochemical Society, Vol. 154, Issue 11, p. A1005-A1009
DOI: 10.1149/1.2776160

Lithium Ion Battery Graphite Solid Electrolyte Interphase Revealed by Microscopy and Spectroscopy
journal, January 2013

Nie, Mengyun; Chalasani, Dinesh; Abraham, Daniel P.
The Journal of Physical Chemistry C, Vol. 117, Issue 3, p. 1257-1267
DOI: 10.1021/jp3118055

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

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