Abstract
Analysis of the performance evolution and failure mechanisms of commercial Li-ion batteries is crucial for improving testing methods, accurately modeling battery performance, and ensuring safe battery operation. Here, we present the results of a 2-year aging study conducted on commercial large-format LiNiMnCoO2-graphite pouch cells. Loss of lithium inventory (LLI) and loss of positive electrode active material (LAMPE) are shown to dominate capacity fade, as quantified by differential voltage-capacity analysis; only a small amount of LAMPE was measured in extracted electrode material, indicating that LAMPE in full cells was due to electrode dry-out. Resistance evolution, observed by direct current pulses and electrochemical impedance spectroscopy analyzed using the distribution of relaxation times, shows complex trends. Particle cracking and electrode expansion is theorized to cause most changes to resistance. Post-mortem measurements reveal a 10% increase in electrode stack thickness and substantial gas generation, with lithium plating observed in extreme cycling conditions, causing large resistance increases. Circumstantial evidence for self-discharge via redox shuttle, which decomposes the electrolyte, is shown. Overall, electrolyte stability was determined to be the limiting factor for cell lifetime. The impacts of many degradation mechanisms on diagnostic signals substantially overlap, making it challenging to monitor cell health and safety.
Original language | American English |
---|---|
Number of pages | 15 |
Journal | Journal of Power Sources |
Volume | 604 |
DOIs | |
State | Published - 2024 |
NREL Publication Number
- NREL/JA-5700-89744
Keywords
- battery degradation
- differential voltage-capacity
- electrochemical impedance spectroscopy
- electrolyte decomposition
- failure analysis
- lithium-ion battery
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Gasper, P., Sunderlin, N., Dunlap, N., Walker, P., Finegan, D., Smith, K., & Thakkar, F. (2024). Lithium Loss, Resistance Growth, Electrode Expansion, Gas Evolution, and Li Plating: Analyzing Performance and Failure of Commercial Large-Format NMC-Gr Lithium-Ion Pouch Cells: Article No. 234494. Journal of Power Sources, 604. https://doi.org/10.1016/j.jpowsour.2024.234494
Gasper, Paul ; Sunderlin, Nathaniel ; Dunlap, Nathan et al. / Lithium Loss, Resistance Growth, Electrode Expansion, Gas Evolution, and Li Plating: Analyzing Performance and Failure of Commercial Large-Format NMC-Gr Lithium-Ion Pouch Cells : Article No. 234494. In: Journal of Power Sources. 2024 ; Vol. 604.
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title = "Lithium Loss, Resistance Growth, Electrode Expansion, Gas Evolution, and Li Plating: Analyzing Performance and Failure of Commercial Large-Format NMC-Gr Lithium-Ion Pouch Cells: Article No. 234494",
abstract = "Analysis of the performance evolution and failure mechanisms of commercial Li-ion batteries is crucial for improving testing methods, accurately modeling battery performance, and ensuring safe battery operation. Here, we present the results of a 2-year aging study conducted on commercial large-format LiNiMnCoO2-graphite pouch cells. Loss of lithium inventory (LLI) and loss of positive electrode active material (LAMPE) are shown to dominate capacity fade, as quantified by differential voltage-capacity analysis; only a small amount of LAMPE was measured in extracted electrode material, indicating that LAMPE in full cells was due to electrode dry-out. Resistance evolution, observed by direct current pulses and electrochemical impedance spectroscopy analyzed using the distribution of relaxation times, shows complex trends. Particle cracking and electrode expansion is theorized to cause most changes to resistance. Post-mortem measurements reveal a 10% increase in electrode stack thickness and substantial gas generation, with lithium plating observed in extreme cycling conditions, causing large resistance increases. Circumstantial evidence for self-discharge via redox shuttle, which decomposes the electrolyte, is shown. Overall, electrolyte stability was determined to be the limiting factor for cell lifetime. The impacts of many degradation mechanisms on diagnostic signals substantially overlap, making it challenging to monitor cell health and safety.",
keywords = "battery degradation, differential voltage-capacity, electrochemical impedance spectroscopy, electrolyte decomposition, failure analysis, lithium-ion battery",
author = "Paul Gasper and Nathaniel Sunderlin and Nathan Dunlap and Patrick Walker and Donal Finegan and Kandler Smith and Foram Thakkar",
year = "2024",
doi = "10.1016/j.jpowsour.2024.234494",
language = "American English",
volume = "604",
journal = "Journal of Power Sources",
issn = "0378-7753",
publisher = "Elsevier",
}
Gasper, P, Sunderlin, N, Dunlap, N, Walker, P, Finegan, D, Smith, K & Thakkar, F 2024, 'Lithium Loss, Resistance Growth, Electrode Expansion, Gas Evolution, and Li Plating: Analyzing Performance and Failure of Commercial Large-Format NMC-Gr Lithium-Ion Pouch Cells: Article No. 234494', Journal of Power Sources, vol. 604. https://doi.org/10.1016/j.jpowsour.2024.234494
Lithium Loss, Resistance Growth, Electrode Expansion, Gas Evolution, and Li Plating: Analyzing Performance and Failure of Commercial Large-Format NMC-Gr Lithium-Ion Pouch Cells: Article No. 234494. / Gasper, Paul; Sunderlin, Nathaniel; Dunlap, Nathan et al.
In: Journal of Power Sources, Vol. 604, 2024.
Research output: Contribution to journal › Article › peer-review
TY - JOUR
T1 - Lithium Loss, Resistance Growth, Electrode Expansion, Gas Evolution, and Li Plating: Analyzing Performance and Failure of Commercial Large-Format NMC-Gr Lithium-Ion Pouch Cells
T2 - Article No. 234494
AU - Gasper, Paul
AU - Sunderlin, Nathaniel
AU - Dunlap, Nathan
AU - Walker, Patrick
AU - Finegan, Donal
AU - Smith, Kandler
AU - Thakkar, Foram
PY - 2024
Y1 - 2024
N2 - Analysis of the performance evolution and failure mechanisms of commercial Li-ion batteries is crucial for improving testing methods, accurately modeling battery performance, and ensuring safe battery operation. Here, we present the results of a 2-year aging study conducted on commercial large-format LiNiMnCoO2-graphite pouch cells. Loss of lithium inventory (LLI) and loss of positive electrode active material (LAMPE) are shown to dominate capacity fade, as quantified by differential voltage-capacity analysis; only a small amount of LAMPE was measured in extracted electrode material, indicating that LAMPE in full cells was due to electrode dry-out. Resistance evolution, observed by direct current pulses and electrochemical impedance spectroscopy analyzed using the distribution of relaxation times, shows complex trends. Particle cracking and electrode expansion is theorized to cause most changes to resistance. Post-mortem measurements reveal a 10% increase in electrode stack thickness and substantial gas generation, with lithium plating observed in extreme cycling conditions, causing large resistance increases. Circumstantial evidence for self-discharge via redox shuttle, which decomposes the electrolyte, is shown. Overall, electrolyte stability was determined to be the limiting factor for cell lifetime. The impacts of many degradation mechanisms on diagnostic signals substantially overlap, making it challenging to monitor cell health and safety.
AB - Analysis of the performance evolution and failure mechanisms of commercial Li-ion batteries is crucial for improving testing methods, accurately modeling battery performance, and ensuring safe battery operation. Here, we present the results of a 2-year aging study conducted on commercial large-format LiNiMnCoO2-graphite pouch cells. Loss of lithium inventory (LLI) and loss of positive electrode active material (LAMPE) are shown to dominate capacity fade, as quantified by differential voltage-capacity analysis; only a small amount of LAMPE was measured in extracted electrode material, indicating that LAMPE in full cells was due to electrode dry-out. Resistance evolution, observed by direct current pulses and electrochemical impedance spectroscopy analyzed using the distribution of relaxation times, shows complex trends. Particle cracking and electrode expansion is theorized to cause most changes to resistance. Post-mortem measurements reveal a 10% increase in electrode stack thickness and substantial gas generation, with lithium plating observed in extreme cycling conditions, causing large resistance increases. Circumstantial evidence for self-discharge via redox shuttle, which decomposes the electrolyte, is shown. Overall, electrolyte stability was determined to be the limiting factor for cell lifetime. The impacts of many degradation mechanisms on diagnostic signals substantially overlap, making it challenging to monitor cell health and safety.
KW - battery degradation
KW - differential voltage-capacity
KW - electrochemical impedance spectroscopy
KW - electrolyte decomposition
KW - failure analysis
KW - lithium-ion battery
U2 - 10.1016/j.jpowsour.2024.234494
DO - 10.1016/j.jpowsour.2024.234494
M3 - Article
SN - 0378-7753
VL - 604
JO - Journal of Power Sources
JF - Journal of Power Sources
ER -
Gasper P, Sunderlin N, Dunlap N, Walker P, Finegan D, Smith K et al. Lithium Loss, Resistance Growth, Electrode Expansion, Gas Evolution, and Li Plating: Analyzing Performance and Failure of Commercial Large-Format NMC-Gr Lithium-Ion Pouch Cells: Article No. 234494. Journal of Power Sources. 2024;604. doi: 10.1016/j.jpowsour.2024.234494