Regulating Na content and Mn defects in birnessite for high-voltage aqueous sodium-ion batteries

Xiaohui Zhu, Jing Xu (), Qinghua Zhang, Tao Shen, Yuhang Zhuang, Tingting Chen, Shuang Li (), Lin Gu () and Hui Xia ()
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Xiaohui Zhu: Nanjing University of Science and Technology
Jing Xu: Nanjing University of Science and Technology
Qinghua Zhang: Chinese Academy of Sciences
Tao Shen: Nanjing University of Science and Technology
Yuhang Zhuang: Nanjing University of Science and Technology
Tingting Chen: Nanjing University of Science and Technology
Shuang Li: Nanjing University of Science and Technology
Lin Gu: Tsinghua University
Hui Xia: Nanjing University of Science and Technology

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: Abstract Na-birnessite is a promising low-cost positive electrode material for aqueous sodium-ion batteries. However, its sodium storage capability is limited by narrow potential window and low redox activity in aqueous electrolytes. Herein, a Na-rich birnessite (NaMnO2•0.1H2O) with a highly ordered layered structure is reported as an advanced positive electrode for aqueous sodium-ion batteries, greatly suppressing Mn migration and its accompanying domino degradation effect, which enables a promoted upper charging cut-off potential up to 1.4 V (vs. Ag/AgCl), an enhanced specific capacity of 199.9 mAh g−1 at a specific current of 0.2 A g−1 based on the mass of active material for positive electrode, and greatly improved structural stability. In particular, a 3.0 V NaxH2–xTi2O5||NaMnO2•0.1H2O aqueous full cell prototype is validated, exhibiting a large specific energy of 117.1 Wh kg−1 based on the total mass of active materials in both positive and negative electrodes as well as a long cycle life. This work elucidates how interlayer chemistry and structural defects influence sodium ion storage in layered structures and provides opportunities for developing high-voltage aqueous batteries with large specific energy.

Date: 2025
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DOI: 10.1038/s41467-025-59223-1

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