Coupling of Oxygen Dimer and Trapped O2 with Strong Magnetic Frustration in Layered Li-rich Cathodes

Xiang Wu; Xiaobing Lou; Chunjing Hu; Fushan Geng; Jingxin Li; Chao Li; Bingwen Hu

doi:10.1021/acsenergylett.4c02919

Coupling of Oxygen Dimer and Trapped O₂ with Strong Magnetic Frustration in Layered Li-rich Cathodes

Xiang Wu
, Xiaobing Lou
, Chunjing Hu
, Fushan Geng
, Jingxin Li
, Chao Li
, Bingwen Hu^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

7 Scopus citations

Abstract

Anion redox in layered Li-rich cathodes provides a high capacity but triggers a series of cascading issues. Current research predominantly focuses on how oxygen species participate in redox and how transition metals move, often ignoring the influence of magnetic frustration. This work systematically investigates the potential link between the evolution of magnetic frustration, structural evolution and oxygen redox in honeycomb Li₂RuO₃. Our findings indicate that the phase transition from C2/c to R3 exacerbates the magnetic frustration during Ru oxidation. Subsequently, during oxygen oxidation, the strong magnetic frustration drives the generation of (O₂)ⁿ⁻ and trapped O₂, which serves to relieve and eventually eliminate the magnetic frustration. This (O₂)ⁿ⁻/O₂ formation mechanism, termed “magnetic-frustration-driven mechanism”, provides a plausible explanation for the formation of trapped O₂ in the systems with strong covalent TM-O bonds. Accordingly, we emphasize that improvement strategies should not only enhance the covalent TM-O bonds but also relieve strong magnetic frustration.

Original language	English
Pages (from-to)	459-468
Number of pages	10
Journal	ACS Energy Letters
Volume	10
Issue number	1
DOIs	https://doi.org/10.1021/acsenergylett.4c02919
State	Published - 10 Jan 2025
Externally published	Yes

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title = "Coupling of Oxygen Dimer and Trapped O2 with Strong Magnetic Frustration in Layered Li-rich Cathodes",

abstract = "Anion redox in layered Li-rich cathodes provides a high capacity but triggers a series of cascading issues. Current research predominantly focuses on how oxygen species participate in redox and how transition metals move, often ignoring the influence of magnetic frustration. This work systematically investigates the potential link between the evolution of magnetic frustration, structural evolution and oxygen redox in honeycomb Li2RuO3. Our findings indicate that the phase transition from C2/c to R3 exacerbates the magnetic frustration during Ru oxidation. Subsequently, during oxygen oxidation, the strong magnetic frustration drives the generation of (O2)n− and trapped O2, which serves to relieve and eventually eliminate the magnetic frustration. This (O2)n−/O2 formation mechanism, termed “magnetic-frustration-driven mechanism”, provides a plausible explanation for the formation of trapped O2 in the systems with strong covalent TM-O bonds. Accordingly, we emphasize that improvement strategies should not only enhance the covalent TM-O bonds but also relieve strong magnetic frustration.",

author = "Xiang Wu and Xiaobing Lou and Chunjing Hu and Fushan Geng and Jingxin Li and Chao Li and Bingwen Hu",

note = "Publisher Copyright: {\textcopyright} 2024 American Chemical Society.",

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doi = "10.1021/acsenergylett.4c02919",

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TY - JOUR

T1 - Coupling of Oxygen Dimer and Trapped O2 with Strong Magnetic Frustration in Layered Li-rich Cathodes

AU - Wu, Xiang

AU - Lou, Xiaobing

AU - Hu, Chunjing

AU - Geng, Fushan

AU - Li, Jingxin

AU - Li, Chao

AU - Hu, Bingwen

PY - 2025/1/10

Y1 - 2025/1/10

N2 - Anion redox in layered Li-rich cathodes provides a high capacity but triggers a series of cascading issues. Current research predominantly focuses on how oxygen species participate in redox and how transition metals move, often ignoring the influence of magnetic frustration. This work systematically investigates the potential link between the evolution of magnetic frustration, structural evolution and oxygen redox in honeycomb Li2RuO3. Our findings indicate that the phase transition from C2/c to R3 exacerbates the magnetic frustration during Ru oxidation. Subsequently, during oxygen oxidation, the strong magnetic frustration drives the generation of (O2)n− and trapped O2, which serves to relieve and eventually eliminate the magnetic frustration. This (O2)n−/O2 formation mechanism, termed “magnetic-frustration-driven mechanism”, provides a plausible explanation for the formation of trapped O2 in the systems with strong covalent TM-O bonds. Accordingly, we emphasize that improvement strategies should not only enhance the covalent TM-O bonds but also relieve strong magnetic frustration.

AB - Anion redox in layered Li-rich cathodes provides a high capacity but triggers a series of cascading issues. Current research predominantly focuses on how oxygen species participate in redox and how transition metals move, often ignoring the influence of magnetic frustration. This work systematically investigates the potential link between the evolution of magnetic frustration, structural evolution and oxygen redox in honeycomb Li2RuO3. Our findings indicate that the phase transition from C2/c to R3 exacerbates the magnetic frustration during Ru oxidation. Subsequently, during oxygen oxidation, the strong magnetic frustration drives the generation of (O2)n− and trapped O2, which serves to relieve and eventually eliminate the magnetic frustration. This (O2)n−/O2 formation mechanism, termed “magnetic-frustration-driven mechanism”, provides a plausible explanation for the formation of trapped O2 in the systems with strong covalent TM-O bonds. Accordingly, we emphasize that improvement strategies should not only enhance the covalent TM-O bonds but also relieve strong magnetic frustration.

UR - https://www.scopus.com/pages/publications/85213206998

U2 - 10.1021/acsenergylett.4c02919

DO - 10.1021/acsenergylett.4c02919

M3 - 文章

AN - SCOPUS:85213206998

SN - 2380-8195

VL - 10

SP - 459

EP - 468

JO - ACS Energy Letters

JF - ACS Energy Letters

IS - 1

ER -

Coupling of Oxygen Dimer and Trapped O₂ with Strong Magnetic Frustration in Layered Li-rich Cathodes

Abstract

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