Twin boundary defect engineering improves lithium-ion diffusion for fast-charging spinel cathode materials

Rui Wang, Xin Chen, Zhongyuan Huang, Jinlong Yang, Fusheng Liu, Mihai Chu, Tongchao Liu, Chaoqi Wang, Weiming Zhu, Shuankui Li, Shunning Li, Jiaxin Zheng, Jie Chen, Lunhua He (), Lei Jin (), Feng Pan () and Yinguo Xiao ()
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Rui Wang: Peking University, Shenzhen Graduate School
Xin Chen: Peking University, Shenzhen Graduate School
Zhongyuan Huang: Peking University, Shenzhen Graduate School
Jinlong Yang: Shenzhen University
Fusheng Liu: Shenzhen University
Mihai Chu: Peking University, Shenzhen Graduate School
Tongchao Liu: Peking University, Shenzhen Graduate School
Chaoqi Wang: Peking University, Shenzhen Graduate School
Weiming Zhu: Peking University, Shenzhen Graduate School
Shuankui Li: Peking University, Shenzhen Graduate School
Shunning Li: Peking University, Shenzhen Graduate School
Jiaxin Zheng: Peking University, Shenzhen Graduate School
Jie Chen: Institute of High Energy Physics, Chinese Academy of Sciences
Lunhua He: Spallation Neutron Source Science Center
Lei Jin: Ernst Ruska-Centre for Microscopy and Spectroscopy with Electrons, Forschungszentrum Jülich GmbH
Feng Pan: Peking University, Shenzhen Graduate School
Yinguo Xiao: Peking University, Shenzhen Graduate School

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: Abstract Defect engineering on electrode materials is considered an effective approach to improve the electrochemical performance of batteries since the presence of a variety of defects with different dimensions may promote ion diffusion and provide extra storage sites. However, manipulating defects and obtaining an in-depth understanding of their role in electrode materials remain challenging. Here, we deliberately introduce a considerable number of twin boundaries into spinel cathodes by adjusting the synthesis conditions. Through high-resolution scanning transmission electron microscopy and neutron diffraction, the detailed structures of the twin boundary defects are clarified, and the formation of twin boundary defects is attributed to agminated lithium atoms occupying the Mn sites around the twin boundary. In combination with electrochemical experiments and first-principles calculations, we demonstrate that the presence of twin boundaries in the spinel cathode enables fast lithium-ion diffusion, leading to excellent fast charging performance, namely, 75% and 58% capacity retention at 5 C and 10 C, respectively. These findings demonstrate a simple and effective approach for fabricating fast-charging cathodes through the use of defect engineering.

Date: 2021
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DOI: 10.1038/s41467-021-23375-7

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