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Title: What makes lithium substituted polyacrylic acid a better binder than polyacrylic acid for silicon-graphite composite anodes?

Abstract

Lithium substituted polyacrylic acid (LiPAA) has previously been demonstrated as a superior binder over polyacrylic acid (PAA) for Si anodes, but from where does this enhanced performance arise? In this paper, full cells are assembled with PAA and LiPAA based Si-graphite composite anodes that dried at temperatures from 100 °C to 200 °C. The performance of full cells containing PAA based Si-graphite anodes largely depend on the secondary drying temperature, as decomposition of the binder is correlated to increased electrode moisture and a rise in cell impedance. Full cells containing LiPAA based Si-graphite composite electrodes display better Coulombic efficiency than those with PAA, because of the electrochemical reduction of the PAA binder. This is identified by attenuated total reflectance Fourier transform infrared spectrometry and observed gassing during the electrochemical reaction. Finally, Coulombic losses from the PAA and Si SEI, along with depletion of the Si capacity in the anode results in progressive underutilization of the cathode and full cell capacity loss.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1];  [2];  [2];  [1]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Energy and Transportation Science Division
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences 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); USDOE Office of Science (SC)
OSTI Identifier:
1424453
Alternate Identifier(s):
OSTI ID: 1548643
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Power Sources
Additional Journal Information:
Journal Volume: 384; Journal ID: ISSN 0378-7753
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Li ion battery; Si graphite anode; polyacrylic acid; lithium substituted polyacrylic acid; full cells; residual water

Citation Formats

Hays, Kevin A., Ruther, Rose E., Kukay, Alexander J., Cao, Pengfei, Saito, Tomonori, Wood, David L., and Li, Jianlin. What makes lithium substituted polyacrylic acid a better binder than polyacrylic acid for silicon-graphite composite anodes?. United States: N. p., 2018. Web. doi:10.1016/j.jpowsour.2018.02.085.
Hays, Kevin A., Ruther, Rose E., Kukay, Alexander J., Cao, Pengfei, Saito, Tomonori, Wood, David L., & Li, Jianlin. What makes lithium substituted polyacrylic acid a better binder than polyacrylic acid for silicon-graphite composite anodes?. United States. doi:10.1016/j.jpowsour.2018.02.085.
Hays, Kevin A., Ruther, Rose E., Kukay, Alexander J., Cao, Pengfei, Saito, Tomonori, Wood, David L., and Li, Jianlin. Sun . "What makes lithium substituted polyacrylic acid a better binder than polyacrylic acid for silicon-graphite composite anodes?". United States. doi:10.1016/j.jpowsour.2018.02.085. https://www.osti.gov/servlets/purl/1424453.
@article{osti_1424453,
title = {What makes lithium substituted polyacrylic acid a better binder than polyacrylic acid for silicon-graphite composite anodes?},
author = {Hays, Kevin A. and Ruther, Rose E. and Kukay, Alexander J. and Cao, Pengfei and Saito, Tomonori and Wood, David L. and Li, Jianlin},
abstractNote = {Lithium substituted polyacrylic acid (LiPAA) has previously been demonstrated as a superior binder over polyacrylic acid (PAA) for Si anodes, but from where does this enhanced performance arise? In this paper, full cells are assembled with PAA and LiPAA based Si-graphite composite anodes that dried at temperatures from 100 °C to 200 °C. The performance of full cells containing PAA based Si-graphite anodes largely depend on the secondary drying temperature, as decomposition of the binder is correlated to increased electrode moisture and a rise in cell impedance. Full cells containing LiPAA based Si-graphite composite electrodes display better Coulombic efficiency than those with PAA, because of the electrochemical reduction of the PAA binder. This is identified by attenuated total reflectance Fourier transform infrared spectrometry and observed gassing during the electrochemical reaction. Finally, Coulombic losses from the PAA and Si SEI, along with depletion of the Si capacity in the anode results in progressive underutilization of the cathode and full cell capacity loss.},
doi = {10.1016/j.jpowsour.2018.02.085},
journal = {Journal of Power Sources},
number = ,
volume = 384,
place = {United States},
year = {2018},
month = {3}
}

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Figures / Tables:

Figure 1 Figure 1: Cycle life of A) LiPAA full cells and B) PAA full cells. The Coulombic efficiency for the first 10 cycles of C) LiPAA full cells and D) PAA full cells. The long term Coulombic efficiency of E) LiPAA full cells and F) PAA full cells. The secondary dryingmore » temperature of the Si-graphite composite anodes are 120 °C (red circle), 140 °C (gold square), 160 °C (green triangle), 180 °C (blue diamond), and 200 °C (black hour glass). Each point is an average of 3 cells.« less

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