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Tuning Oxide Properties by Oxygen Vacancy Control During Growth and Annealing

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Oxygen Dimerization as a Defect-Driven Process in Bulk LiNiO₂.

Alexander G Squires^1,2, Lavan Ganeshkumar^2,3, Christopher N Savory¹

¹School of Chemistry, The University of Birmingham, Edgbaston, Birmingham B15 2TT, United Kingdom.

ACS Energy Letters

|August 15, 2024

Summary

This summary is machine-generated.

Oxygen dimerization in lithium nickel oxide cathode materials is possible, especially at high charge states. Defects in these materials can initiate oxygen dimerization, contributing to bulk degradation.

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Area of Science:

Materials Science
Electrochemistry
Solid-State Chemistry

Background:

Nickel-rich lithium nickel oxide (LiNiO2) is a promising cathode material for lithium-ion batteries.
High states of charge in these materials can lead to oxygen release and degradation.
Conflicting reports exist regarding the formation of molecular oxygen within the bulk of LiNiO2.

Purpose of the Study:

To investigate the potential for oxygen dimerization in the bulk of LiNiO2 cathode materials.
To understand the role of high charge states in oxygen species formation.
To elucidate the mechanisms behind bulk degradation in nickel-rich cathodes.

Main Methods:

Utilized a redox-product structure search methodology.
Inspired by recent advancements in point-defect structure prediction.
Focused on delithiated Li1-xNiO2 at x = 1 (fully delithiated state).

Main Results:

Delithiated LiNiO2 (x = 1) exhibits kinetic stability against decomposition into molecular oxygen.
Point defects within the material can serve as nucleation sites for oxygen dimerization.
Defect chemistry plays a crucial role in initiating bulk degradation pathways.

Conclusions:

Oxygen dimerization can occur in the bulk of LiNiO2, facilitated by defects.
The findings reconcile previous conflicting observations on oxygen formation in nickel-rich cathodes.
Understanding defect chemistry is key to mitigating bulk degradation and improving cathode stability.