Voltage-dependent charge compensation mechanism and cathode electrolyte interface stability of the lithium-ion battery cathode materials LiCoO2 and LiNi1/3Mn1/3Co1/3O2 studied by photoelectron spectroscopy

Mellin, Maximilian; Cherkashinin, Gennady; Mohseni, Elham; Phillips, Robert; Jaegermann, Wolfram; Hofmann, Jan P.

doi:10.1039/d3ta05981b

J. Mater. Chem. A

2024

DOI: 10.1039/d3ta05981b

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Voltage-dependent charge compensation mechanism and cathode electrolyte interface stability of the lithium-ion battery cathode materials LiCoO₂ and LiNi_1/3Mn_1/3Co_1/3O₂ studied by photoelectron spectroscopy

Maximilian Mellin,

Gennady Cherkashinin,

Elham Mohseni

et al.

Abstract: Enhancing the high voltage limit of layered LiTMO2 (TM = 3d transition metal) cathode materials has motivated intensive research on their properties at high states of charge. This led to...

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Cited by 3 publications

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A Strategy for Mitigating Lattice Stress and Enhancing Cycle Stability Through Modulating Transition Metal Redox Sequence

Ma,

Wang,

Tang

et al. 2024

Small Methods

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Modifying the redox properties of transition metals within layered cathode materials represents a pivotal approach in the pursuit of high‐performance cathode materials. The recent research has revealed a novel finding: the introduction of Mg2+ into LiNi1/3Co1/3Mn1/3O2 leads to a shift in the oxidation sequence of transition metals during lithium extraction, with Co3+ supplanting Ni2+ as the primary oxidized species during the initial stages of lithium extraction. This alteration in the lattice constants and volume, among other structural parameters, serves to mitigate lattice stress during the charging and discharging cycles. The abundance of Co4+ during the early stages of lithium extraction effectively curtails structural alterations and the dissolution of transition metal ions, thereby bolstering the material's cyclability. This effect is attributed to the enhanced Ni─O bond strength imparted by Mg2+ doping, which, in concert with Co3+, stabilizes the Li─O structure at the outset of lithium extraction, conferring a thermodynamic advantage to Co3+ for preferential oxidation. The exploration of the underlying mechanism of this induced effect and its influence on electrochemical performance holds the potential to offer fresh perspectives for the design of materials with exceptional cycle stability.

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A Strategy for Mitigating Lattice Stress and Enhancing Cycle Stability Through Modulating Transition Metal Redox Sequence

Ma,

Wang,

Tang

et al. 2024

Small Methods

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DBD-air-plasma fabrication of N-doped Li-CoO substrate for loading Ag to promote the successive adsorption and oxidation of airborne HCHO

Liu,

Zhang,

Lian

et al. 2025

Applied Surface Science

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In Vacuo Scratching Yields Undisturbed Insight into the Bulk of Lithium-Ion Battery Positive Electrode Materials

Mellin,

Cherkashinin,

Jaegermann

et al. 2024

ACS Energy Lett.

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Characterizing Li-ion battery (LIB) materials by X-ray photoelectron spectroscopy (XPS) poses challenges for sample preparation. This holds especially true for assessing the electronic structure of both the bulk and interphase of positive electrode materials, which involves sample extraction from a battery test cell, sample preparation, and mounting. Here, we introduce the method of in vacuo scratching as preparation for XPS measurements of LIB positive electrode materials, which can drastically reduce spectral contaminations and enhance spectral quality, enabling higher information gain. The benefits of this effective yet simple method are highlighted in comparison to Ar + -sputtering and air contact using commercially applied powder LiNi 1/3 Mn 1/3 Co 1/3 O 2 (NMC333) as showcase material. For assessing interphase formation, the electrode material was soaked in electrolyte, and the effects of rinsing and in vacuo scratching were studied. This treatment results in high signal-to-noise spectra, yielding well-defined photoelectron spectra without the influence of the interphases and spectral artifacts from, e.g., Ar + sputtering.

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Voltage-dependent charge compensation mechanism and cathode electrolyte interface stability of the lithium-ion battery cathode materials LiCoO₂ and LiNi_1/3Mn_1/3Co_1/3O₂ studied by photoelectron spectroscopy

Abstract: Enhancing the high voltage limit of layered LiTMO2 (TM = 3d transition metal) cathode materials has motivated intensive research on their properties at high states of charge. This led to...

Cited by 3 publications

References 65 publications

A Strategy for Mitigating Lattice Stress and Enhancing Cycle Stability Through Modulating Transition Metal Redox Sequence

A Strategy for Mitigating Lattice Stress and Enhancing Cycle Stability Through Modulating Transition Metal Redox Sequence

DBD-air-plasma fabrication of N-doped Li-CoO substrate for loading Ag to promote the successive adsorption and oxidation of airborne HCHO

In Vacuo Scratching Yields Undisturbed Insight into the Bulk of Lithium-Ion Battery Positive Electrode Materials

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