Volume 9, Issue 7 2401868
Research Article

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

Yushan Ma

Yushan Ma

College of Chemistry and Chemical Engineering, Central South University, Changsha, 410083 China

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Jinkun Wang

Jinkun Wang

Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing, 100084 China

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Xincun Tang

Corresponding Author

Xincun Tang

College of Chemistry and Chemical Engineering, Central South University, Changsha, 410083 China

E-mail: [email protected]; [email protected]

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Li Wang

Li Wang

Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing, 100084 China

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Xiangming He

Corresponding Author

Xiangming He

Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing, 100084 China

E-mail: [email protected]; [email protected]

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First published: 23 December 2024

Abstract

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.

Conflict of Interest

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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