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

Kezhu Jiang; Shaohua Guo; Wei Kong Pang; Xueping Zhang; Tiancheng Fang; Shao fei Wang; Fangwei Wang; Xiaoyu Zhang; Ping He; Haoshen Zhou

doi:10.1007/s12274-021-3349-4

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

Kezhu Jiang, Shaohua Guo, Wei Kong Pang, Xueping Zhang, Tiancheng Fang, Shao fei Wang, Fangwei Wang, Xiaoyu Zhang, Ping He, Haoshen Zhou

Research output: Contribution to journal › Article › peer-review

40 Scopus citations

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 Na_0.9Ni_0.3Co_0.15Mn_0.05Ti_0.5O₂ 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. [Figure not available: see fulltext.].

Original language	English
Pages (from-to)	4100-4106
Number of pages	7
Journal	Nano Research
Volume	14
Issue number	11
DOIs	https://doi.org/10.1007/s12274-021-3349-4
State	Published - Nov 2021
Externally published	Yes

Funding

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).

Funders	Funder number
CSNS
National Institute of Standards and Technology
Australian Research Council	FT160100251
National Natural Science Foundation of China	U1801251, 51802149, 22075132
Nanjing University
Fundamental Research Funds for the Central Universities

Keywords

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

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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Cite this

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title = "Oxygen vacancy promising highly reversible phase transition in layered cathodes for sodium-ion batteries",

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. [Figure not available: see fulltext.].",

keywords = "O3 phase, layered oxide, oxygen vacancy, reversible phase transition, sodium-ion battery",

author = "Kezhu Jiang and Shaohua Guo and Pang, {Wei Kong} and Xueping Zhang and Tiancheng Fang and Wang, {Shao fei} and Fangwei Wang and Xiaoyu Zhang and Ping He and Haoshen Zhou",

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AU - Zhang, Xueping

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AU - Zhang, Xiaoyu

AU - He, Ping

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AB - 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. [Figure not available: see fulltext.].

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

Abstract

Funding

Keywords

UN SDGs

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