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Multi-scale synergistic regulation of hierarchical porous Ni@NiSe cathodes with low voltage gap, high capacity and long-term cycling stability in Li–CO2 battery

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Abstract

The Li–CO2 battery often suffers from high overpotential and limited capacity due to the challenges associated with the adsorption of Li+ and CO2 and the decomposition of Li2CO3. Herein, hexagonal rich-stepped NiSe crystals are in situ achieved on a three-dimensional (3D) free-standing porous Ni skeleton with double continuous channel architecture (namely p-Ni@NiSe-50) through an in situ selenization process. Structural characterization and theoretical calculation are applied to demonstrate the synergistic effects of marco/microstructural design and electronic band structure regulation. As a result, the adsorption/desorption of Li+ and CO2 and the formation/decomposition of Li2CO3 are effectively promoted, simultaneously, enabling an enhanced capacity and reversibility of p-Ni@NiSe-50 as the cathode of Li–CO2 battery. An ultra-low overpotential of 0.46 V and a remarkably high energy efficiency of 83.8% (20 μA cm−2) are achieved, along with a high full discharge specific capacity of 8844 μAh cm−2. Excellent long-term cycling stability (cycles up to 1000 h at a voltage gap of 1.14 V) of p-Ni@NiSe-50 is also obtained. The results of this work would provide a new insight and strategy to develop high-performance alkali metal-air batteries.

Graphical abstract

Multi-scale synergistic effect of combining the cathode macroscopic structure design and the microscopic band structure design of NiSe was demonstrated to promote the adsorption of Li+ and CO2, as well as the decomposition of Li2CO3, so as to achieve ultra-low voltage gap and high capacity of Li-CO2 batteries.

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Data availability

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (51801135) and Ningbo JS Brothers Tool Factory Ltd. (2022GKF-0523). We also thank Ms. Y. Han, Dr. J. Mao, Dr. J. Zhang and Ms. L. Ma from the National Demonstration Center for Materials Science & Engineering Education, Tianjin University for their help and kind advice about the SEM, TEM, and XPS characterization of the samples.

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Authors and Affiliations

  1. School of Materials Science and Engineering and Tianjin Key Laboratory of Composites and Functional Materials, Tianjin University, Tianjin, 300350, China

    Yating Shi, Haonan Xie, Liying Ma, Biao Chen, Jianli Kang, Chunsheng Shi, Chunnian He & Junwei Sha

  2. Collaborative Innovation Center of Chemical Science and Engineering, Tianjin, 300350, China

    Chunnian He

  3. Key Laboratory of Advanced Ceramics and Machining Technology, Ministry of Education, Tianjin, 300350, China

    Chunnian He

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  1. Yating Shi
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Contributions

Yating Shi involved in investigation, methodology, data curation, and writing—original draft. Haonan Xie involved in methodology and data curation. Liying Ma involved in data curation. Biao Chen involved in methodology. Jianli Kang involved in data curation. Chunsheng Shi involved in data curation. Chunnian He involved in writing—review and editing. Junwei Sha involved in supervision, methodology, data curation, funding acquisition, and writing—review and editing.

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Shi, Y., Xie, H., Ma, L. et al. Multi-scale synergistic regulation of hierarchical porous Ni@NiSe cathodes with low voltage gap, high capacity and long-term cycling stability in Li–CO2 battery. J Mater Sci 59, 12613–12629 (2024). https://doi.org/10.1007/s10853-024-09922-9

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