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 (2025)

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 languageAmerican English
Number of pages15
JournalJournal of Power Sources
Volume604
DOIs
StatePublished - 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",

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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, 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 journalArticlepeer-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

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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.

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KW - electrochemical impedance spectroscopy

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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

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 (2025)
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