Three-dimensional atomic-scale observation of structural evolution of cathode material in a working all-solid-state battery

被引：73

作者：

Gong, Yue ^{[1
,2
]}

Chen, Yuyang ^{[1
,2
]}

Zhang, Qinghua ^{[1
]}

Meng, Fanqi ^{[1
,2
]}

Shi, Jin-An ^{[1
,2
]}

Liu, Xinyu ^{[1
,2
]}

Liu, Xiaozhi ^{[1
,2
]}

Zhang, Jienan ^{[1
,2
]}

Wang, Hao ^{[1
,2
]}

Wang, Jiangyong ^{[3
]}

Yu, Qian ^{[4
,5
]}

Zhang, Ze ^{[4
,5
]}

Xu, Qiang ^{[6
]}

Xiao, Ruijuan ^{[1
]}

Hu, Yong-Sheng ^{[1
]}

Gu, Lin ^{[1
,2
,7
]}

Li, Hong ^{[1
]}

Huang, Xuejie ^{[1
]}

Chen, Liquan ^{[1
]}

机构：

[1] Chinese Acad Sci, Inst Phys, Beijing Natl Lab Condensed Matter Phys, Beijing 100190, Peoples R China

[2] Univ Chinese Acad Sci, Sch Phys Sci, Beijing 100049, Peoples R China

[3] Shantou Univ, Dept Phys, Shantou 515063, Guangdong, Peoples R China

[4] Zhejiang Univ, Ctr Electron Microscopy, Hangzhou 310027, Zhejiang, Peoples R China

[5] Zhejiang Univ, Sch Mat Sci & Engn, State Key Lab Silicon Mat, Hangzhou 310027, Zhejiang, Peoples R China

[6] DENSsolutions, Informaticalaan 12, NL-2628 ZD Delft, Netherlands

[7] Collaborat Innovat Ctr Quantum Matter, Beijing 100084, Peoples R China

来源：

NATURE COMMUNICATIONS | 2018年 / 9卷

基金：

中国国家自然科学基金; 北京市自然科学基金;

关键词：

DENSITY-FUNCTIONAL THEORY; TOTAL-ENERGY CALCULATIONS; IN-SITU; LINI0.5MN1.5O4; CATHODE; PHASE-TRANSFORMATION; ELECTRONIC-STRUCTURE; CYCLING PERFORMANCE; KINETIC-PROPERTIES; MN3+ CONTENT; SURFACE;

D O I：

10.1038/s41467-018-05833-x

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

Most technologically important electrode materials for lithium-ion batteries are essentially lithium ions plus a transition-metal oxide framework. However, their atomic and electronic structure evolution during electrochemical cycling remains poorly understood. Here we report the in situ observation of the three-dimensional structural evolution of the transition-metal oxide framework in an all-solid-state battery. The in situ studies LiNi0.5Mn1.5O4 from various zone axes reveal the evolution of both atomic and electronic structures during delithiation, which is found due to the migration of oxygen and transition-metal ions. Ordered to disordered structural transition proceeds along the <100>, <110>, <111> directions and inhomogeneous structural evolution along the <112> direction. Uneven extraction of lithium ions leads to localized migration of transition-metal ions and formation of antiphase boundaries. Dislocations facilitate transition-metal ions migration as well. Theoretical calculations suggest that doping of lower valence-state cations effectively stabilize the structure during delithiation and inhibit the formation of boundaries.

引用

页数：8

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