Single-Crystallization of O3-Type Layered Oxide Cathode for Na-Ion Battery

The development of high-energy-density Na-ion batteries places significant demands on single-crystal layered oxide cathodes, especially for further high-voltage, solid-state battery scenarios. In the O3-type structure, due to the original sluggish Na ion diffusion kinetics (approximately 1 order of magnitude lower than that of Li-ion), and further hindrance against diffusion kinetics caused by single-crystal architecture, these inherent defects lead to the decline in the electrochemical performance. Herein, we demonstrated that the single crystallization of O3-type NaNi1/3Fe1/3Mn1/3O2 cathode (d50 = 5.04 μm) aggravates surface-to-bulk phase inhomogeneity distribution, which is attributed to the uneven Na ions extraction. Moreover, the Na-depletion of the surface/shell region not only aggravates Na ion diffusion resistance but also leads to a higher valence state of transition-metal elements (e.g., Ni/Fe) near the surface of the single-crystal particle, which further compromises the cathode-electrolyte interface stability. Not limited to revealing the challenges, tuning the particle size and moderating quasi-single-crystal strategies have been proven to effectively mitigate the negative uneven distributions of Na ions, phases, and valence/oxidative states, resulting in efficient modification for single crystallization of Na-layered oxide cathodes.

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Publication Details

Journal
Chemistry of Materials
Published
2025-07-19
DOI
https://doi.org/10.1021/acs.chemmater.5c01106
Citations
2
Primary Topic
Advancements in Battery Materials
Type
article
Field-Weighted Citation Impact
1.46

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article

Single-Crystallization of O3-Type Layered Oxide Cathode for Na-Ion Battery

Yonglin Tang, Kai Fang, Gui‐Liang Xu, Qirui Liu et al.
2 citations
Chemistry of Materials
Advancements in Battery Materials
1.46
article

Single-Crystallization of O3-Type Layered Oxide Cathode for Na-Ion Battery

Yonglin Tang, Kai Fang, Gui‐Liang Xu, Qirui Liu, Yuhao Hong, Ziyang Ning, Khalil Amine, Wenhua Zuo, Chuying Ouyang, Guifan Zeng, Niu Liu, Tian Qiu, Qiaobao Zhang, Zhefei Sun, Jiarui Li, Kang Zhang, Yu Qiao, Shi‐Gang Sun, Xianghui Xiao, Dongyan Yu
article en
2 citations

Abstract

The development of high-energy-density Na-ion batteries places significant demands on single-crystal layered oxide cathodes, especially for further high-voltage, solid-state battery scenarios. In the O3-type structure, due to the original sluggish Na ion diffusion kinetics (approximately 1 order of magnitude lower than that of Li-ion), and further hindrance against diffusion kinetics caused by single-crystal architecture, these inherent defects lead to the decline in the electrochemical performance. Herein, we demonstrated that the single crystallization of O3-type NaNi1/3Fe1/3Mn1/3O2 cathode (d50 = 5.04 μm) aggravates surface-to-bulk phase inhomogeneity distribution, which is attributed to the uneven Na ions extraction. Moreover, the Na-depletion of the surface/shell region not only aggravates Na ion diffusion resistance but also leads to a higher valence state of transition-metal elements (e.g., Ni/Fe) near the surface of the single-crystal particle, which further compromises the cathode-electrolyte interface stability. Not limited to revealing the challenges, tuning the particle size and moderating quasi-single-crystal strategies have been proven to effectively mitigate the negative uneven distributions of Na ions, phases, and valence/oxidative states, resulting in efficient modification for single crystallization of Na-layered oxide cathodes.

Chemistry of MaterialsVol. 37(15)
Argonne National Laboratory (US), Xiamen University (CN), Brookhaven National Laboratory (US), Stanford Synchrotron Radiation Lightsource (US), Shanghai Huayi Group (China) (CN), Tan Kah Kee Innovation Laboratory (CN), Collaborative Innovation Center of Chemistry for Energy Materials (CN), National Synchrotron Light Source II
U.S. Department of Energy, National Natural Science Foundation of China, Ministry of Science and Technology of the People's Republic of China
Openalex Percentile: Top 16%
Advancements in Battery Materials
1.46
DOISourceOpenAlex
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