Transition metal vacancy and position engineering enables reversible anionic redox reaction for sodium storage
Abstract Triggering the anionic redox reaction is an effective approach to boost the capacity of layered transition metal (TM) oxides. However, the irreversible oxygen release and structural deterioration at high voltage remain conundrums. Herein, a strategy for Mg ion and vacancy dual doping with p...
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Nature Portfolio
2025-01-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-54998-1 |
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| author | Congcong Cai Xinyuan Li Jiantao Li Ruohan Yu Ping Hu Ting Zhu Tianyi Li Sungsik Lee Nuo Xu Hao Fan Jinsong Wu Liang Zhou Liqiang Mai Khalil Amine |
| author_facet | Congcong Cai Xinyuan Li Jiantao Li Ruohan Yu Ping Hu Ting Zhu Tianyi Li Sungsik Lee Nuo Xu Hao Fan Jinsong Wu Liang Zhou Liqiang Mai Khalil Amine |
| author_sort | Congcong Cai |
| collection | DOAJ |
| description | Abstract Triggering the anionic redox reaction is an effective approach to boost the capacity of layered transition metal (TM) oxides. However, the irreversible oxygen release and structural deterioration at high voltage remain conundrums. Herein, a strategy for Mg ion and vacancy dual doping with partial TM ions pinned in the Na layers is developed to improve both the reversibility of anionic redox reaction and structural stability of layered oxides. Both the Mg ions and vacancies (□) are contained in the TM layers, while partial Mn ions (~1.1%) occupy the Na-sites. The introduced Mg ions combined with vacancies not only create abundant nonbonding O 2p orbitals in favor of high oxygen redox capacity, but also suppress the voltage decay originated from Na–O–□ configuration. The Mn ions pinned in the Na layers act as “rivets” to restrain the slab gliding at extreme de-sodiated state and thereby inhibit the generation of cracks. The positive electrode, Na0.67Mn0.011[Mg0.1□0.07Mn0.83]O2, delivers an enhanced discharge capacity and decent cyclability. This study provides insights into the construction of stable layered oxide positive electrode with highly reversible anionic redox reaction for sodium storage. |
| format | Article |
| id | doaj-art-8ebe8f4ed5294dec92927639d440c1a3 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-8ebe8f4ed5294dec92927639d440c1a32025-01-05T12:38:57ZengNature PortfolioNature Communications2041-17232025-01-0116111210.1038/s41467-024-54998-1Transition metal vacancy and position engineering enables reversible anionic redox reaction for sodium storageCongcong Cai0Xinyuan Li1Jiantao Li2Ruohan Yu3Ping Hu4Ting Zhu5Tianyi Li6Sungsik Lee7Nuo Xu8Hao Fan9Jinsong Wu10Liang Zhou11Liqiang Mai12Khalil Amine13State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of TechnologyState Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of TechnologyChemical Sciences and Engineering Division, Argonne National LaboratoryState Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of TechnologyState Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of TechnologyState Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of TechnologyX-ray Science Division, Advanced Photon Source, Argonne National LaboratoryX-ray Science Division, Advanced Photon Source, Argonne National LaboratoryState Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of TechnologyState Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of TechnologyState Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of TechnologyState Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of TechnologyState Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of TechnologyChemical Sciences and Engineering Division, Argonne National LaboratoryAbstract Triggering the anionic redox reaction is an effective approach to boost the capacity of layered transition metal (TM) oxides. However, the irreversible oxygen release and structural deterioration at high voltage remain conundrums. Herein, a strategy for Mg ion and vacancy dual doping with partial TM ions pinned in the Na layers is developed to improve both the reversibility of anionic redox reaction and structural stability of layered oxides. Both the Mg ions and vacancies (□) are contained in the TM layers, while partial Mn ions (~1.1%) occupy the Na-sites. The introduced Mg ions combined with vacancies not only create abundant nonbonding O 2p orbitals in favor of high oxygen redox capacity, but also suppress the voltage decay originated from Na–O–□ configuration. The Mn ions pinned in the Na layers act as “rivets” to restrain the slab gliding at extreme de-sodiated state and thereby inhibit the generation of cracks. The positive electrode, Na0.67Mn0.011[Mg0.1□0.07Mn0.83]O2, delivers an enhanced discharge capacity and decent cyclability. This study provides insights into the construction of stable layered oxide positive electrode with highly reversible anionic redox reaction for sodium storage.https://doi.org/10.1038/s41467-024-54998-1 |
| spellingShingle | Congcong Cai Xinyuan Li Jiantao Li Ruohan Yu Ping Hu Ting Zhu Tianyi Li Sungsik Lee Nuo Xu Hao Fan Jinsong Wu Liang Zhou Liqiang Mai Khalil Amine Transition metal vacancy and position engineering enables reversible anionic redox reaction for sodium storage Nature Communications |
| title | Transition metal vacancy and position engineering enables reversible anionic redox reaction for sodium storage |
| title_full | Transition metal vacancy and position engineering enables reversible anionic redox reaction for sodium storage |
| title_fullStr | Transition metal vacancy and position engineering enables reversible anionic redox reaction for sodium storage |
| title_full_unstemmed | Transition metal vacancy and position engineering enables reversible anionic redox reaction for sodium storage |
| title_short | Transition metal vacancy and position engineering enables reversible anionic redox reaction for sodium storage |
| title_sort | transition metal vacancy and position engineering enables reversible anionic redox reaction for sodium storage |
| url | https://doi.org/10.1038/s41467-024-54998-1 |
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