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Title: Lithium and transition metal dissolution due to aqueous processing in lithium-ion battery cathode active materials

Abstract

Enabling aqueous processing for lithium-ion battery cathodes is essential as solvents like N-methyl-2-pyrrolidone (NMP) are expensive, hazardous, and being phased out of usage around the world. Using water as a solvent can reduce electrode manufacturing cost and environmental impact, but it presents unique challenges for cathodes such as Li and transition metal dissolution from the active material and current collector corrosion. In this study, the suitability of aqueous processing for five cathode active materials is evaluated, specifically: LiCoO2 (LCO), LiFePO4 (LFP), LiMn2O4 (LMO), LiNi0.80Co0.15Al0.05O2 (NCA), and LiNi0.5Mn0.3Co0.2O2 (NMC532). After three days of water exposure, NCA and NMC532 exhibit significantly greater pH values (11.5–12.5) than the Ni-free materials (9.0–10.5), though all pH values suggest corrosion of the Al substrate would occur. Surface compositions change to various extent while little change is observed in the crystal structures. The transition metal dissolution in water and electrolyte is relatively low for all materials, though the Li dissolution in water is high for NCA (~0.1 mg mL-1). Electrochemical testing in half coin cells reveals that high-molecular weight polyacrylic acid addition is able to modify the pH and provide adequate binding to the current collector to permit aqueous processing of NCA.

Authors:
 [1];  [1];  [2]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [1]
+ Show Author Affiliations
  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. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
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:
1619030
Alternate Identifier(s):
OSTI ID: 1618026
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Power Sources
Additional Journal Information:
Journal Volume: 466; Journal Issue: C; Journal ID: ISSN 0378-7753
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Lithium-ion battery; Aqueous electrode processing; NCA cathode; Lithium leaching; Cation exchange; Cycle life

Citation Formats

Hawley, William Blake, Parejiya, Anand Vasudevbhai, Bai, Yaocai, Meyer III, Harry M., Wood III, David L., and Li, Jianlin. Lithium and transition metal dissolution due to aqueous processing in lithium-ion battery cathode active materials. United States: N. p., 2020. Web. doi:10.1016/j.jpowsour.2020.228315.
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Hawley, William Blake, Parejiya, Anand Vasudevbhai, Bai, Yaocai, Meyer III, Harry M., Wood III, David L., & Li, Jianlin. Lithium and transition metal dissolution due to aqueous processing in lithium-ion battery cathode active materials. United States. https://doi.org/10.1016/j.jpowsour.2020.228315
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Hawley, William Blake, Parejiya, Anand Vasudevbhai, Bai, Yaocai, Meyer III, Harry M., Wood III, David L., and Li, Jianlin. Fri . "Lithium and transition metal dissolution due to aqueous processing in lithium-ion battery cathode active materials". United States. https://doi.org/10.1016/j.jpowsour.2020.228315. https://www.osti.gov/servlets/purl/1619030.
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@article{osti_1619030,
title = {Lithium and transition metal dissolution due to aqueous processing in lithium-ion battery cathode active materials},
author = {Hawley, William Blake and Parejiya, Anand Vasudevbhai and Bai, Yaocai and Meyer III, Harry M. and Wood III, David L. and Li, Jianlin},
abstractNote = {Enabling aqueous processing for lithium-ion battery cathodes is essential as solvents like N-methyl-2-pyrrolidone (NMP) are expensive, hazardous, and being phased out of usage around the world. Using water as a solvent can reduce electrode manufacturing cost and environmental impact, but it presents unique challenges for cathodes such as Li and transition metal dissolution from the active material and current collector corrosion. In this study, the suitability of aqueous processing for five cathode active materials is evaluated, specifically: LiCoO2 (LCO), LiFePO4 (LFP), LiMn2O4 (LMO), LiNi0.80Co0.15Al0.05O2 (NCA), and LiNi0.5Mn0.3Co0.2O2 (NMC532). After three days of water exposure, NCA and NMC532 exhibit significantly greater pH values (11.5–12.5) than the Ni-free materials (9.0–10.5), though all pH values suggest corrosion of the Al substrate would occur. Surface compositions change to various extent while little change is observed in the crystal structures. The transition metal dissolution in water and electrolyte is relatively low for all materials, though the Li dissolution in water is high for NCA (~0.1 mg mL-1). Electrochemical testing in half coin cells reveals that high-molecular weight polyacrylic acid addition is able to modify the pH and provide adequate binding to the current collector to permit aqueous processing of NCA.},
doi = {10.1016/j.jpowsour.2020.228315},
journal = {Journal of Power Sources},
number = C,
volume = 466,
place = {United States},
year = {Fri May 08 00:00:00 EDT 2020},
month = {Fri May 08 00:00:00 EDT 2020}
}
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https://doi.org/10.1016/j.jpowsour.2020.228315
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