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Native Vacancy Enhanced Oxygen Redox Reversibility and Structural Robustness

机译：原始空缺增强了氧气的氧化还原可逆性和结构稳健性

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摘要

Cathode materials with high energy density, long cycle life, and low cost are of top priority for energy storage systems. The Li-rich transition metal (TM) oxides achieve high specific capacities by redox reactions of both the TM and oxygen ions. However, the poor reversible redox reaction of the anions results in severe fading of the cycling performance. Herein, the vacancy-containing Na-4/7[Mn-6/7(◻(Mn))(1/7)]O-2 (◻(Mn) for vacancies in the Mn Symbol of the Klingon Empire O slab) is presented as a novel cathode material for Na-ion batteries. The presence of native vacancies endows this material with attractive properties including high structural flexibility and stability upon Na-ion extraction and insertion and high reversibility of oxygen redox reaction. Synchrotron X-ray absorption near edge structure and X-ray photoelectron spectroscopy studies demonstrate that the charge compensation is dominated by the oxygen redox reaction and Mn3+/Mn4+ redox reaction separately. In situ synchrotron X-ray diffraction exhibits its zero-strain feature during the cycling. Density functional theory calculations further deepen the understanding of the charge compensation by oxygen and manganese redox reactions and the immobility of the Mn ions in the material. These findings provide new ideas on searching for and designing materials with high capacity and high structural stability for novel energy storage systems.
机译：具有高能量密度，长循环寿命和低成本的阴极材料是储能系统的重中之重。富锂的过渡金属（TM）氧化物通过TM和氧离子的氧化还原反应实现高比容量。但是，不良的阴离子可逆氧化还原反应导致循环性能严重下降。在此，含有空位的Na-4 / 7 [Mn-6 / 7（◻（Mn））（1/7）] O-2（在克林贡帝国O板的Mn符号中为◻的Mn（Mn））作为一种用于Na离子电池的新型阴极材料，被提出。天然空位的存在使该材料具有诱人的性能，包括在Na离子萃取和插入时具有高结构柔性和稳定性，以及氧还原反应的高可逆性。同步加速器在边缘结构附近的X射线吸收和X射线光电子能谱研究表明，电荷补偿分别由氧氧化还原反应和Mn3 + / Mn4 +氧化还原反应控制。在循环过程中，原位同步加速器X射线衍射显示出零应变特征。密度泛函理论计算进一步加深了对氧和锰氧化还原反应的电荷补偿以及材料中Mn离子固定性的理解。这些发现为寻找和设计用于新型储能系统的高容量和高结构稳定性的材料提供了新思路。

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  • 来源
    《Advanced energy materials》 |2019年第4期|1803087.1-1803087.9|共9页
  • 作者

    Li Yejing; Wang Xuefeng; Gao Yurui; Zhang Qinghua; Tan Guoqiong; Kong Qingyu; Bak Seongmin; Lu Gang; Yang Xiao-Qing; Gu Lin; Lu Jun; Amine Khalil; Wang Zhaoxiang; Chen Liquan;

  • 作者单位

    Chinese Acad Sci, Inst Phys, Key Lab Renewable Energy, POB 603, Beijing 100190, Peoples R China|Univ Chinese Acad Sci, Sch Phys Sci, POB 603, Beijing 100190, Peoples R China;

    Chinese Acad Sci, Inst Phys, Key Lab Renewable Energy, POB 603, Beijing 100190, Peoples R China|Univ Calif San Diego, Dept NanoEngn, 9500 Gilman Dr, La Jolla, CA 92093 USA;

    Calif State Univ Northridge, Dept Phys & Astron, Northridge, CA 91330 USA;

    Chinese Acad Sci, Inst Phys, Lab Adv Mat & Electron Microscopy, POB 603, Beijing 100190, Peoples R China;

    Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Lemont, IL 60439 USA;

    Synchrotron Soleil, F-91192 Gif Sur Yvette, France;

    Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA;

    Calif State Univ Northridge, Dept Phys & Astron, Northridge, CA 91330 USA;

    Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA;

    Chinese Acad Sci, Inst Phys, Lab Adv Mat & Electron Microscopy, POB 603, Beijing 100190, Peoples R China;

    Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Lemont, IL 60439 USA;

    Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Lemont, IL 60439 USA;

    Chinese Acad Sci, Inst Phys, Key Lab Renewable Energy, POB 603, Beijing 100190, Peoples R China|Univ Chinese Acad Sci, Sch Phys Sci, POB 603, Beijing 100190, Peoples R China;

    Chinese Acad Sci, Inst Phys, Key Lab Renewable Energy, POB 603, Beijing 100190, Peoples R China|Univ Chinese Acad Sci, Sch Phys Sci, POB 603, Beijing 100190, Peoples R China;

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  • 正文语种 eng
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  • 关键词

    cathode materials; charge compensation; oxygen redox; sodium manganese oxide; zero-strain;

    机译：正极材料;电荷补偿;氧化还原;钠锰氧化物;零应变;

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