Achieving High‐Capacity Cathode Presodiation Agent Via Triggering Anionic Oxidation Activity in Sodium Oxide

Author:

Chen Yilong12,Zhu Yuanlong1,Sun Zhefei3,Kuai Xiaoxiao12,Chen Jianken1,Zhang Baodan1,Yin Jianhua1,Luo Haiyan1,Tang Yonglin1,Zeng Guifan1,Zhang Kang1,Li Li1,Xu Juping45,Yin Wen45,Qiu Yongfu6,Zou Yeguo12,Ning Ziyang7,Ouyang Chuying78,Zhang Qiaobao3,Qiao Yu12ORCID,Sun Shi‐Gang1

Affiliation:

1. State Key Laboratory of Physical Chemistry of Solid Surfaces Department of Chemistry College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 China

2. Fujian Science & Technology Innovation Laboratory for Energy Materials of China (Tan Kah Kee Innovation Laboratory) Xiamen 361005 China

3. State Key Laboratory of Physical Chemistry of Solid Surfaces College of Materials Xiamen University Xiamen 361005 China

4. Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 China

5. Spallation Neutron Source Science Center Dongguan 523803 China

6. School of Materials Science and Engineering Dongguan University of Technology Guangdong 523808 China

7. Fujian Science & Technology Innovation Laboratory for Energy Devices (21C‐Lab) Contemporary Amperex Technology Co., Limited (CATL) Ningde 352100 China

8. Department of Physics Laboratory of Computational Materials Physics Jiangxi Normal University Nanchang 330022 China

Abstract

AbstractCompensating for the irreversible loss of limited active sodium (Na) is crucial for enhancing the energy density of practical sodium‐ion batteries (SIBs) full‐cell, especially when employing hard carbon anode with initially lower coulombic efficiency. Introducing sacrificial cathode presodiation agents, particularly those that own potential anionic oxidation activity with a high theoretical capacity, can provide additional sodium sources for compensating Na loss. Herein, Ni atoms are precisely implanted at the Na sites within Na2O framework, obtaining a (Na0.89Ni0.050.06)2O (Ni–Na2O) presodiation agent. The synergistic interaction between Na vacancies and Ni catalyst effectively tunes the band structure, forming moderate Ni–O covalent bonds, activating the oxidation activity of oxygen anion, reducing the decomposition overpotential to 2.8 V (vs Na/Na+), and achieving a high presodiation capacity of 710 mAh/g≈Na2O (Na2O decomposition rate >80%). Incorporating currently‐modified presodiation agent with Na3V2(PO4)3 and Na2/3Ni2/3Mn1/3O2 cathodes, the energy density of corresponding Na‐ion full‐cells presents an essential improvement of 23.9% and 19.3%, respectively. Further, not limited to Ni–Na2O, the structure–function relationship between the anionic oxidation mechanism and electrode–electrolyte interface fabrication is revealed as a paradigm for the development of sacrificial cathode presodiation agent.

Funder

National Natural Science Foundation of China

Fundamental Research Funds for the Central Universities

Ministry of Science and Technology of the People's Republic of China

Publisher

Wiley

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