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

W. Blake Hawley; Anand Parejiya; Yaocai Bai; Harry M. Meyer; David L. Wood; Jianlin Li

doi:10.1016/j.jpowsour.2020.228315

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

W. Blake Hawley, Anand Parejiya, Yaocai Bai, Harry M. Meyer, David L. Wood, Jianlin Li

Research output: Contribution to journal › Article › peer-review

79 Scopus citations

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: LiCoO₂ (LCO), LiFePO₄ (LFP), LiMn₂O₄ (LMO), LiNi_0.80Co_0.15Al_0.05O₂ (NCA), and LiNi_0.5Mn_0.3Co_0.2O₂ (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.

Original language	English
Article number	228315
Journal	Journal of Power Sources
Volume	466
DOIs	https://doi.org/10.1016/j.jpowsour.2020.228315
State	Published - Aug 1 2020

Funding

This manuscript has been authored in part by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. The DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan).This research at Oak Ridge National Laboratory (ORNL), managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) under contract DE-AC05-00OR22725, was sponsored by the Office of Energy Efficiency and Renewable Energy (EERE) Vehicle Technologies Office (VTO) (Director: David Howell; Applied Battery Research (ABR) Program Manager: Peter Faguy). The authors acknowledge Tamara Keever (ORNL) for her assistance with ICP-MS analysis and Ritu Sahore (ORNL) for her aid in reviewing the manuscript. This manuscript has been authored in part by UT-Battelle, LLC , under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. The DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ). This research at Oak Ridge National Laboratory (ORNL), managed by UT Battelle, LLC, for the U.S. Department of Energy ( DOE ) under contract DE-AC05-00OR22725, was sponsored by the Office of Energy Efficiency and Renewable Energy ( EERE ) Vehicle Technologies Office ( VTO ) (Director: David Howell; Applied Battery Research (ABR) Program Manager: Peter Faguy). The authors acknowledge Tamara Keever (ORNL) for her assistance with ICP-MS analysis and Ritu Sahore (ORNL) for her aid in reviewing the manuscript.

Funders	Funder number
DOE Public Access Plan
Tamara Keever
US Department of Energy
U.S. Department of Energy	DE-AC05-00OR22725
Battelle
Office of Energy Efficiency and Renewable Energy
Oak Ridge National Laboratory
Vehicle Technologies Office
UT-Battelle

Keywords

Aqueous electrode processing
Cation exchange
Cycle life
Lithium leaching
Lithium-ion battery
NCA cathode

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1016/j.jpowsour.2020.228315

Cite this

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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: 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.",

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AU - Parejiya, Anand

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AU - Wood, David L.

AU - Li, Jianlin

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AB - 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: 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.

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KW - Cycle life

KW - Lithium leaching

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

Abstract

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Keywords

UN SDGs

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