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Title: Electrolyte Reactivity at the Charged Ni-Rich Cathode Interface and Degradation in Li-Ion Batteries

Abstract

The chemical and electrochemical reactions at the positive electrode–electrolyte interface in Li-ion batteries are hugely influential on cycle life and safety. Ni-rich layered transition metal oxides exhibit higher interfacial reactivity than their lower Ni-content analogues, reacting via mechanisms that are poorly understood. Here, we study the pivotal role of the electrolyte solvent, specifically cyclic ethylene carbonate (EC) and linear ethyl methyl carbonate (EMC), in determining the interfacial reactivity at charged LiNi0.33Mn0.33Co0.33O2 (NMC111) and LiNi0.8Mn0.1Co0.1O2 (NMC811) cathodes by using both single-solvent model electrolytes and the mixed solvents used in commercial cells. While NMC111 exhibits similar parasitic currents with EC-containing and EC-free electrolytes during high voltage holds in NMC/Li4Ti5O12 (LTO) cells, this is not the case for NMC811. Online gas analysis reveals that the solvent-dependent reactivity for Ni-rich cathodes is related to the extent of lattice oxygen release and accompanying electrolyte decomposition, which is higher for EC-containing than EC-free electrolytes. Combined findings from electrochemical impedance spectroscopy (EIS), TEM, solution NMR, ICP, and XPS reveal that the electrolyte solvent has a profound impact on the degradation of the Ni-rich cathode and the electrolyte. Higher lattice oxygen release with EC-containing electrolytes is coupled with higher cathode interfacial impedance, a thicker oxygen-deficient rock-salt surface reconstructionmore » layer, more electrolyte solvent and salt breakdown, and higher amounts of transition metal dissolution. These processes are suppressed in the EC-free electrolyte, highlighting the incompatibility between Ni-rich cathodes and conventional electrolyte solvents. Finally, new mechanistic insights into the chemical oxidation pathways of electrolyte solvents and, critically, the knock-on chemical and electrochemical reactions that further degrade the electrolyte and electrodes curtailing battery lifetime are provided.« less

Authors:
ORCiD logo [1];  [2];  [1];  [3];  [1];  [4]; ORCiD logo [4]; ORCiD logo [3];  [1]; ORCiD logo [1]
+ Show Author Affiliations
  1. Univ. of Cambridge (United Kingdom); The Faraday Institution (United Kingdom)
  2. Univ. of Cambridge (United Kingdom)
  3. The Faraday Institution (United Kingdom); Univ. of Oxford (United Kingdom)
  4. The Faraday Institution (United Kingdom); Univ. of Liverpool (United Kingdom)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States). Cell Analysis, Modeling and Prototyping (CAMP) Facility
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1981987
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 14; Journal Issue: 11; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; lithium-ion batteries; degradation; Ni-rich cathode; NMC; electrolyte reactivity; ethylene carbonate; ethyl methyl carbonate; lattice oxygen

Citation Formats

Dose, Wesley M., Temprano, Israel, Allen, Jennifer P., Björklund, Erik, O’Keefe, Christopher A., Li, Weiqun, Mehdi, B. Layla, Weatherup, Robert S., De Volder, Michael F. L., and Grey, Clare P. Electrolyte Reactivity at the Charged Ni-Rich Cathode Interface and Degradation in Li-Ion Batteries. United States: N. p., 2022. Web. doi:10.1021/acsami.1c22812.
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Dose, Wesley M., Temprano, Israel, Allen, Jennifer P., Björklund, Erik, O’Keefe, Christopher A., Li, Weiqun, Mehdi, B. Layla, Weatherup, Robert S., De Volder, Michael F. L., & Grey, Clare P. Electrolyte Reactivity at the Charged Ni-Rich Cathode Interface and Degradation in Li-Ion Batteries. United States. https://doi.org/10.1021/acsami.1c22812
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Dose, Wesley M., Temprano, Israel, Allen, Jennifer P., Björklund, Erik, O’Keefe, Christopher A., Li, Weiqun, Mehdi, B. Layla, Weatherup, Robert S., De Volder, Michael F. L., and Grey, Clare P. Tue . "Electrolyte Reactivity at the Charged Ni-Rich Cathode Interface and Degradation in Li-Ion Batteries". United States. https://doi.org/10.1021/acsami.1c22812. https://www.osti.gov/servlets/purl/1981987.
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@article{osti_1981987,
title = {Electrolyte Reactivity at the Charged Ni-Rich Cathode Interface and Degradation in Li-Ion Batteries},
author = {Dose, Wesley M. and Temprano, Israel and Allen, Jennifer P. and Björklund, Erik and O’Keefe, Christopher A. and Li, Weiqun and Mehdi, B. Layla and Weatherup, Robert S. and De Volder, Michael F. L. and Grey, Clare P.},
abstractNote = {The chemical and electrochemical reactions at the positive electrode–electrolyte interface in Li-ion batteries are hugely influential on cycle life and safety. Ni-rich layered transition metal oxides exhibit higher interfacial reactivity than their lower Ni-content analogues, reacting via mechanisms that are poorly understood. Here, we study the pivotal role of the electrolyte solvent, specifically cyclic ethylene carbonate (EC) and linear ethyl methyl carbonate (EMC), in determining the interfacial reactivity at charged LiNi0.33Mn0.33Co0.33O2 (NMC111) and LiNi0.8Mn0.1Co0.1O2 (NMC811) cathodes by using both single-solvent model electrolytes and the mixed solvents used in commercial cells. While NMC111 exhibits similar parasitic currents with EC-containing and EC-free electrolytes during high voltage holds in NMC/Li4Ti5O12 (LTO) cells, this is not the case for NMC811. Online gas analysis reveals that the solvent-dependent reactivity for Ni-rich cathodes is related to the extent of lattice oxygen release and accompanying electrolyte decomposition, which is higher for EC-containing than EC-free electrolytes. Combined findings from electrochemical impedance spectroscopy (EIS), TEM, solution NMR, ICP, and XPS reveal that the electrolyte solvent has a profound impact on the degradation of the Ni-rich cathode and the electrolyte. Higher lattice oxygen release with EC-containing electrolytes is coupled with higher cathode interfacial impedance, a thicker oxygen-deficient rock-salt surface reconstruction layer, more electrolyte solvent and salt breakdown, and higher amounts of transition metal dissolution. These processes are suppressed in the EC-free electrolyte, highlighting the incompatibility between Ni-rich cathodes and conventional electrolyte solvents. Finally, new mechanistic insights into the chemical oxidation pathways of electrolyte solvents and, critically, the knock-on chemical and electrochemical reactions that further degrade the electrolyte and electrodes curtailing battery lifetime are provided.},
doi = {10.1021/acsami.1c22812},
journal = {ACS Applied Materials and Interfaces},
number = 11,
volume = 14,
place = {United States},
year = {Tue Mar 08 00:00:00 EST 2022},
month = {Tue Mar 08 00:00:00 EST 2022}
}
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