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作者:

Yan, Pengfei (Yan, Pengfei.) (学者:闫鹏飞) | Zheng, Jianming (Zheng, Jianming.) | Tang, Zhen-Kun (Tang, Zhen-Kun.) | Devaraj, Arun (Devaraj, Arun.) | Chen, Guoying (Chen, Guoying.) | Amine, Khalil (Amine, Khalil.) | Zhang, Ji-Guang (Zhang, Ji-Guang.) | Liu, Li-Min (Liu, Li-Min.) | Wang, Chongmin (Wang, Chongmin.)

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摘要:

Surfaces, interfaces and grain boundaries are classically known to be sinks of defects generated within the bulk lattice. Here, we report an inverse case by which the defects generated at the particle surface are continuously pumped into the bulk lattice. We show that, during operation of a rechargeable battery, oxygen vacancies produced at the surfaces of lithium-rich layered cathode particles migrate towards the inside lattice. This process is associated with a high cutoff voltage at which an anionic redox process is activated. First-principle calculations reveal that triggering of this redox process leads to a sharp decrease of both the formation energy of oxygen vacancies and the migration barrier of oxidized oxide ions, therefore enabling the migration of oxygen vacancies into the bulk lattice of the cathode. This work unveils a coupled redox dynamic that needs to be taken into account when designing high-capacity layered cathode materials for high-voltage lithium-ion batteries.

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作者机构:

  • [ 1 ] [Yan, Pengfei]Pacific Northwest Natl Lab, Environm Mol Sci Lab, Richland, WA 99352 USA
  • [ 2 ] [Devaraj, Arun]Pacific Northwest Natl Lab, Environm Mol Sci Lab, Richland, WA 99352 USA
  • [ 3 ] [Wang, Chongmin]Pacific Northwest Natl Lab, Environm Mol Sci Lab, Richland, WA 99352 USA
  • [ 4 ] [Yan, Pengfei]Beijing Univ Technol, Inst Microstruct & Properties Adv Mat, Beijing Key Lab Microstruct & Properties Solids, Beijing, Peoples R China
  • [ 5 ] [Zheng, Jianming]Pacific Northwest Natl Lab, Energy & Environm Directorate, Richland, WA 99352 USA
  • [ 6 ] [Zhang, Ji-Guang]Pacific Northwest Natl Lab, Energy & Environm Directorate, Richland, WA 99352 USA
  • [ 7 ] [Tang, Zhen-Kun]Hengyang Normal Univ, Coll Phys & Elect Engn, Hengyang, Peoples R China
  • [ 8 ] [Tang, Zhen-Kun]Beihang Univ, Sch Phys, Beijing, Peoples R China
  • [ 9 ] [Liu, Li-Min]Beihang Univ, Sch Phys, Beijing, Peoples R China
  • [ 10 ] [Chen, Guoying]Lawrence Berkeley Natl Lab, Energy Storage & Distributed Resources Div, Berkeley, CA USA
  • [ 11 ] [Amine, Khalil]Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA

通讯作者信息:

  • 闫鹏飞

    [Yan, Pengfei]Pacific Northwest Natl Lab, Environm Mol Sci Lab, Richland, WA 99352 USA;;[Wang, Chongmin]Pacific Northwest Natl Lab, Environm Mol Sci Lab, Richland, WA 99352 USA;;[Yan, Pengfei]Beijing Univ Technol, Inst Microstruct & Properties Adv Mat, Beijing Key Lab Microstruct & Properties Solids, Beijing, Peoples R China;;[Liu, Li-Min]Beihang Univ, Sch Phys, Beijing, Peoples R China

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来源 :

NATURE NANOTECHNOLOGY

ISSN: 1748-3387

年份: 2019

期: 6

卷: 14

页码: 602-,

3 8 . 3 0 0

JCR@2022

ESI学科: MATERIALS SCIENCE;

ESI高被引阀值:79

JCR分区:1

被引次数:

WoS核心集被引频次: 335

SCOPUS被引频次: 336

ESI高被引论文在榜: 0 展开所有

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