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

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.

doi:10.1021/acsami.1c22812

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

Journal Article · Mon Mar 07 23:00:00 EST 2022 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.1c22812· OSTI ID:1981987

^[1]; Temprano, Israel ^[2]; Allen, Jennifer P. ^[1]; Björklund, Erik ^[3]; O’Keefe, Christopher A. ^[1]; Li, Weiqun ^[4]; ^[4]; ^[3]; De Volder, Michael F. L. ^[1]; ^[1]

Univ. of Cambridge (United Kingdom); The Faraday Institution (United Kingdom)
Univ. of Cambridge (United Kingdom)
The Faraday Institution (United Kingdom); Univ. of Oxford (United Kingdom)
The Faraday Institution (United Kingdom); Univ. of Liverpool (United Kingdom)

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 LiNi_0.33Mn_0.33Co_0.33O₂ (NMC111) and LiNi_0.8Mn_0.1Co_0.1O₂ (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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Cell Analysis, Modeling and Prototyping (CAMP) Facility

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1981987

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 11 Vol. 14; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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