Research Article


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

Kezhu Jiang1, Shaohua Guo1 (✉), Wei Kong Pang2, Xueping Zhang1, Tiancheng Fang1, Shao-fei Wang3,4, Fangwei Wang5,6,7, Xiaoyu Zhang8 (✉), Ping He1, and Haoshen Zhou1,9 (✉)

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1 Center of Energy Storage Materials & Technology, College of Engineering and Applied Sciences, National Laboratory of Solid State Microstructures, Collaborative Innovation Center of Advanced Microstructures, Jiangsu Key Laboratory of Artificial Functional Materials, Nanjing University, Nanjing 210093, China2 Institute for Superconducting & Electronic Materials, School of Mechanical, Materials and Mechatronics Engineering, University of Wollongong, Wollongong, NSW 2522, Australia3 China Spallatoin Neutron Source, Institute of High Energy Physics, Chinese Academy of Sciences, Dongguan 523808, China4 School of Nuclear Science and Technology, University of Chinese Academy of Sciences, Beijing 101408, China5 Beijing National Laboratory for Condensed Matter Physics Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China6 School of Physical Sciences, University of Chinese Academy of Sciences, Beijing 101408, China7 Songshan Lake Materials Laboratory, Dongguan 523808, China8 School of materials science and engineering, Jiangsu University, Zhenjiang 212013, China9 Energy Technology Research Institute, National Institute of Advanced Industrial Science and Technology (AIST), Umezono 1-1-1, Tsukuba, 305-8568, Japan

Keywords: sodium-ion battery, layered oxide, O3 phase, oxygen vacancy, reversible phase transition
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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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Oxygen vacancy promising highly reversible phase transition in layered cathodes for sodium-ion batteries. Nano Res.

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