Direct atomic-scale confirmation of three-phase storage mechanism in Li4Ti5O12 anodes for room-temperature sodium-ion batteries

Yang Sun, Liang Zhao, Huilin Pan, Xia Lu, Lin Gu (), Yong-Sheng Hu (), Hong Li, Michel Armand, Yuichi Ikuhara, Liquan Chen and Xuejie Huang
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Yang Sun: Key Laboratory for Renewable Energy, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences
Liang Zhao: Key Laboratory for Renewable Energy, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences
Huilin Pan: Key Laboratory for Renewable Energy, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences
Xia Lu: Key Laboratory for Renewable Energy, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences
Lin Gu: Laboratory for Advanced Materials & electron Microscopy, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences
Yong-Sheng Hu: Key Laboratory for Renewable Energy, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences
Hong Li: Key Laboratory for Renewable Energy, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences
Michel Armand: Key Laboratory for Renewable Energy, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences
Yuichi Ikuhara: WPI Advanced Institute for Materials Research, Tohoku University
Liquan Chen: Key Laboratory for Renewable Energy, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences
Xuejie Huang: Key Laboratory for Renewable Energy, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences

Nature Communications, 2013, vol. 4, issue 1, 1-10

Abstract: Abstract Room-temperature sodium-ion batteries attract increasing attention for large-scale energy storage applications in renewable energy and smart grid. However, the development of suitable anode materials remains a challenging issue. Here we demonstrate that the spinel Li4Ti5O12, well-known as a ‘zero-strain’ anode for lithium-ion batteries, can also store sodium, displaying an average storage voltage of 0.91 V. With an appropriate binder, the Li4Ti5O12 electrode delivers a reversible capacity of 155 mAh g−1 and presents the best cyclability among all reported oxide-based anode materials. Density functional theory calculations predict a three-phase separation mechanism, 2Li4Ti5O12+6Na++6e−↔Li7Ti5O12+Na6LiTi5O12, which has been confirmed through in situ synchrotron X-ray diffraction and advanced scanning transmission electron microscope imaging techniques. The three-phase separation reaction has never been seen in any insertion electrode materials for lithium- or sodium-ion batteries. Furthermore, interfacial structure is clearly resolved at an atomic scale in electrochemically sodiated Li4Ti5O12 for the first time via the advanced electron microscopy.

Date: 2013
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DOI: 10.1038/ncomms2878

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