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作者:

Zhou, Ke (Zhou, Ke.) | Li, Yining (Li, Yining.) | Zheng, Shiyao (Zheng, Shiyao.) | Zhang, Maojie (Zhang, Maojie.) | Zhang, Chunyang (Zhang, Chunyang.) | Battaglia, Corsin (Battaglia, Corsin.) | Liu, Haodong (Liu, Haodong.) | Wang, Kuan (Wang, Kuan.) | Yan, Pengfei (Yan, Pengfei.) (学者:闫鹏飞) | Liu, Jianjun (Liu, Jianjun.) | Yang, Yong (Yang, Yong.)

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EI Scopus SCIE

摘要:

Lithium-excess cation-disordered rock-salt oxides (DRXs) are investigated intensively as cathode materials for future lithium-ion batteries combining cationic and anionic redox reactions. However, the lattice oxygen redox can cause severe oxygen release resulting in rapid capacity fading. Here, we investigate a series of xLi(2)TiO(3)-(1 - x)LiMnO2 (0 <= x <= 1) materials and find that only Li1.2Mn0.4Ti0.4O2 (x = 0.4) and Li1.1Mn0.7Ti0.2O2 (x = 0.2) can form phase-pure DRXs, which both deliver high capacity (250 mAh g(-1)). The newly discovered Li1.1Mn0.7Ti0.2O2 DRX exhibits remarkably high capacity retention of 84.4% after 20 cycles compared to only 60.8% for Li1.2Mn0.4Ti0.4O2. Our result indicates that the irreversible oxygen loss is reduced by raising the Mn content. Theoretical calculations further reveal that increasing the redox-active Mn content from Li1.2Mn0.4Ti0.4O2 to Li1.1Mn0.7Ti0.2O2 causes the orbitals near the Fermi level to change from O(2)p non-bonding (Li-O-Li unhybridized orbitals) to (Mn-O)* antibonding bands, exhibiting a high O-O aggregation barrier, preventing O-2 release and resulting in sustained capacity retention. Hence, these new findings demonstrate that regulating oxygen redox by tailoring the redox-active transition metal content is an effective strategy to enhance the cycling stability of DRXs.

关键词:

Redox mechanism Cycling stability Cation-disordered rock-salt oxides Electronic structure Redox-active transition metal

作者机构:

  • [ 1 ] [Zhou, Ke]Xiamen Univ, Coll Chem & Chem Engn, Dept Chem, Xiamen 361005, Peoples R China
  • [ 2 ] [Zhang, Maojie]Xiamen Univ, Coll Chem & Chem Engn, Dept Chem, Xiamen 361005, Peoples R China
  • [ 3 ] [Yang, Yong]Xiamen Univ, Coll Chem & Chem Engn, Dept Chem, Xiamen 361005, Peoples R China
  • [ 4 ] [Zhou, Ke]Xiamen Univ, Coll Chem & Chem Engn, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Peoples R China
  • [ 5 ] [Zhang, Maojie]Xiamen Univ, Coll Chem & Chem Engn, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Peoples R China
  • [ 6 ] [Yang, Yong]Xiamen Univ, Coll Chem & Chem Engn, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Peoples R China
  • [ 7 ] [Li, Yining]Empa, Swiss Fed Labs Mat Sci & Technol, CH-8600 Dubendorf, Switzerland
  • [ 8 ] [Zheng, Shiyao]Chinese Acad Sci, Shanghai Inst Ceram, State Key Lab High Performance Ceram & Superfine, Shanghai 200050, Peoples R China
  • [ 9 ] [Liu, Jianjun]Chinese Acad Sci, Shanghai Inst Ceram, State Key Lab High Performance Ceram & Superfine, Shanghai 200050, Peoples R China
  • [ 10 ] [Liu, Jianjun]Penn State Univ, Dept Mech & Nucl Engn, University Pk, PA 16802 USA
  • [ 11 ] [Liu, Haodong]Ecole Polytechn Federale Lausanne, Dept Chem & Chem Engn, Lab Photon & Interfaces, CH-1015 Lausanne, Switzerland
  • [ 12 ] [Wang, Kuan]Univ Calif San Diego, Ctr Memory & Recording Res, La Jolla, CA 92093 USA
  • [ 13 ] [Yan, Pengfei]Univ Calif San Diego, Ctr Memory & Recording Res, La Jolla, CA 92093 USA
  • [ 14 ] [Yang, Yong]Beijing Univ Technol, Fac Mat & Mfg, Beijing Key Lab Microstructure & Properties Solid, Beijing 100124, Peoples R China
  • [ 15 ] [Yang, Yong]Xiamen Univ, Sch Energy, Xiamen 361005, Peoples R China

通讯作者信息:

  • [Yang, Yong]Xiamen Univ, Coll Chem & Chem Engn, Dept Chem, Xiamen 361005, Peoples R China;;[Yang, Yong]Xiamen Univ, Coll Chem & Chem Engn, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Peoples R China;;[Liu, Jianjun]Chinese Acad Sci, Shanghai Inst Ceram, State Key Lab High Performance Ceram & Superfine, Shanghai 200050, Peoples R China;;[Liu, Jianjun]Penn State Univ, Dept Mech & Nucl Engn, University Pk, PA 16802 USA;;[Yang, Yong]Beijing Univ Technol, Fac Mat & Mfg, Beijing Key Lab Microstructure & Properties Solid, Beijing 100124, Peoples R China

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来源 :

ENERGY STORAGE MATERIALS

ISSN: 2405-8297

年份: 2021

卷: 43

页码: 275-283

2 0 . 4 0 0

JCR@2022

JCR分区:1

被引次数:

WoS核心集被引频次: 15

SCOPUS被引频次: 16

ESI高被引论文在榜: 0 展开所有

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