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Nano Research 2021, 14(11): 4100-4106 https://doi.org/10.1007/s12274-021-3349-4
Research Article | Issue | Published: 10 February 2021

Oxygen vacancy promising highly reversible phase transition in layered cathodes for sodium-ion batteries

Show Author's Information Kezhu Jiang1,  Shaohua Guo1( ),  Wei Kong Pang2,  Xueping Zhang1,  Tiancheng Fang1,  Shao-fei Wang3,4,  Fangwei Wang5,6,7,  Xiaoyu Zhang8( ),  Ping He1,  Haoshen Zhou1,9( )
Center of Energy Storage Materials & Technology, College of Engineering and Applied Sciences National Laboratory of Solid State MicrostructuresCollaborative Innovation Center of Advanced MicrostructuresJiangsu Key Laboratory of Artificial Functional Materials, Nanjing UniversityNanjing 210093 China
Institute for Superconducting & Electronic Materials, School of Mechanical, Materials and Mechatronics Engineering, University of Wollongong Wollongong, NSW 2522 Australia
China Spallatoin Neutron Source Institute of High Energy Physics, Chinese Academy of SciencesDongguan 523808 China
School of Nuclear Science and Technology University of Chinese Academy of SciencesBeijing 101408 China
Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of SciencesBeijing 100190 China
School of Physical Sciences University of Chinese Academy of SciencesBeijing 101408 China
Songshan Lake Materials LaboratoryDongguan 523808 China
School of materials science and engineering Jiangsu UniversityZhenjiang 212013 China
Energy Technology Research Institute, National Institute of Advanced Industrial Science and Technology (AIST) Umezono 1-1-1Tsukuba 305-8568 Japan
Keywords:
oxygen vacancy, sodium-ion battery, layered oxide, O3 phase, reversible phase transition
Topics:
CathodesCobalt compoundsIon batteriesManganese compoundsMetal ionsNickel compoundsSodiumSodium compoundsTitanium compoundsTransition metals
Cite this article:
Jiang K, Guo S, Pang WK, et al. Oxygen vacancy promising highly reversible phase transition in layered cathodes for sodium-ion batteries. Nano Research, 2021, 14(11): 4100-4106. https://doi.org/10.1007/s12274-021-3349-4
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Abstract Full text Electronic supplementary material About this article

Phase transition is common during (de)-intercalating layered sodium oxides, which directly affects the structural stability and electrochemical performance. However, the artificial control of phase transition to achieve advanced sodium-ion batteries is lacking, since the remarkably little is known about the influencing factor relative to the sliding process of transition-metal slabs upon sodium release and uptake of layered oxides. Herein, we for the first time demonstrate the manipulation of oxygen vacancy concentrations in multinary metallic oxides has a significant impact on the reversibility of phase transition, thereby determining the sodium storage performance of cathode materials. Results show that abundant oxygen vacancies intrigue the return of the already slide transition-metal slabs between O3 and P3 phase transition, in contrast to the few oxygen vacancies and resulted irreversibility. Additionally, the abundant oxygen vacancies enhance the electronic and ionic conductivity of the Na0.9Ni0.3Co0.15Mn0.05Ti0.5O2 electrode, delivering the high initial Coulombic efficiency of 97.1%, large reversible capacity of 112.7 mAh∙g−1, superior rate capability upon 100 C and splendid cycling performance over 1, 000 cycles. Our findings open up new horizons for artificially manipulating the structural evolution and electrochemical process of layered cathodes, and pave a way in designing advanced sodium-ion batteries.


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Abstract
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Electronic supplementary material
About this article

Oxygen vacancy promising highly reversible phase transition in layered cathodes for sodium-ion batteries

Show Author's information Kezhu Jiang1, Shaohua Guo1( ), Wei Kong Pang2, Xueping Zhang1, Tiancheng Fang1, Shao-fei Wang3,4, Fangwei Wang5,6,7, Xiaoyu Zhang8( ), Ping He1, Haoshen Zhou1,9( )
Center of Energy Storage Materials & Technology, College of Engineering and Applied Sciences National Laboratory of Solid State MicrostructuresCollaborative Innovation Center of Advanced MicrostructuresJiangsu Key Laboratory of Artificial Functional Materials, Nanjing UniversityNanjing 210093 China
Institute for Superconducting & Electronic Materials, School of Mechanical, Materials and Mechatronics Engineering, University of Wollongong Wollongong, NSW 2522 Australia
China Spallatoin Neutron Source Institute of High Energy Physics, Chinese Academy of SciencesDongguan 523808 China
School of Nuclear Science and Technology University of Chinese Academy of SciencesBeijing 101408 China
Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of SciencesBeijing 100190 China
School of Physical Sciences University of Chinese Academy of SciencesBeijing 101408 China
Songshan Lake Materials LaboratoryDongguan 523808 China
School of materials science and engineering Jiangsu UniversityZhenjiang 212013 China
Energy Technology Research Institute, National Institute of Advanced Industrial Science and Technology (AIST) Umezono 1-1-1Tsukuba 305-8568 Japan

Abstract

Phase transition is common during (de)-intercalating layered sodium oxides, which directly affects the structural stability and electrochemical performance. However, the artificial control of phase transition to achieve advanced sodium-ion batteries is lacking, since the remarkably little is known about the influencing factor relative to the sliding process of transition-metal slabs upon sodium release and uptake of layered oxides. Herein, we for the first time demonstrate the manipulation of oxygen vacancy concentrations in multinary metallic oxides has a significant impact on the reversibility of phase transition, thereby determining the sodium storage performance of cathode materials. Results show that abundant oxygen vacancies intrigue the return of the already slide transition-metal slabs between O3 and P3 phase transition, in contrast to the few oxygen vacancies and resulted irreversibility. Additionally, the abundant oxygen vacancies enhance the electronic and ionic conductivity of the Na0.9Ni0.3Co0.15Mn0.05Ti0.5O2 electrode, delivering the high initial Coulombic efficiency of 97.1%, large reversible capacity of 112.7 mAh∙g−1, superior rate capability upon 100 C and splendid cycling performance over 1, 000 cycles. Our findings open up new horizons for artificially manipulating the structural evolution and electrochemical process of layered cathodes, and pave a way in designing advanced sodium-ion batteries.

Keywords: oxygen vacancy, sodium-ion battery, layered oxide, O3 phase, reversible phase transition

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Publication history
Copyright
Acknowledgements

Publication history

Received: 14 December 2020
Revised: 13 January 2021
Accepted: 19 January 2021
Published: 10 February 2021
Issue date: November 2021

Copyright

© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021

Acknowledgements

Acknowledgements

The financial is supported by the National Natural Science Foundation of China (Nos. 22075132, 51802149, and U1801251), the Fundamental Research Funds for the Central Universities, and Nanjing University Technology Innovation Fund Project. The authors are also grateful to the High Performance Computing Center (HPCC) of Nanjing University for doing the numerical calculations in this paper on its blade cluster system. W. K. P. is grateful to the financial support by the Australian Research Council through a Future Fellowship project (No. FT160100251). The operational support of ANSTO staffs, especially Dr. Vanessa Peterson and Dr. Christophe Didier, on the collection of neutron powder diffraction data of NaNCMT is highly appreciated. The neutron diffraction data were collected at ANSTO (Australia), CSNS (China), and NIST (USA).

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