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Facilitating polysulfide confinement using N-doped honeycomb-like carbon with high pyridinic-nitrogen content for high-performance Li-S batteries

高吡啶氮含量的氮掺杂蜂窝状碳促进对多硫化物的 限制以实现高性能锂硫电池

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Abstract

Increasing the amount of the nitrogen dopant, especially pyridinic-N species, in carbonaceous materials has been shown to significantly enhance the performance of lithium-sulfur (Li-S) batteries. Despite the positive impact of N do** on carbonaceous materials, the practical realisation of a high N dopant content of >5 at.% remains a significant challenge. Furthermore, to regulate the specific N species in carbonaceous materials is another hurdle. Herein, we obtained a three-dimensional honeycomb-like N-doped mesoporous carbon (PNMC) material with a high N dopant content of 8.82 at.% (pyridinic-N content, 3.49 at.%) by calcining calcium pantothenate under an Ar atmosphere after a phosphorisation process. It is believed that the P dopant contributes to the enhancement of not only the N content but also the polysulfide adsorption capability of the N dopant. As expected, the sulfur cathode comprising PNMC prepared at 800°C (S/PNMC-800) exhibited superior electrochemical performance as confirmed by the discharge specific capacity of 556.7 mA h g−1 observed after 300 cycles at 1 C. This study proposes a facile regulation technique to dope pyridinic-N species in carbonaceous materials, which may trigger the future inventive development of functional S hosts for use in Li-S batteries.

摘要

提高碳材料中氮的掺杂含量, 尤其是吡啶氮的含量, 已被证明可 以显著提升锂硫(Li-S)电池的性能. 尽管在碳材料中氮掺杂具有积极作 用, 但在实际操作中要实现>5 at.%的高氮掺杂含量仍非易事. 此外, 无 法调节碳材料中特定的氮种类也是研究中的一个难题. 在本文中, 我们 通过在氩气气氛下煅烧预先经过磷化处理的泛酸钙, 得到了一种三维 蜂窝状的氮(N)掺杂介孔碳(PNMC), 其N掺杂含量高达8.82 at.%(吡啶 N含量为3.49 at.%). 磷掺杂不仅有助于提高N掺杂量, 还有助于提升对 多硫化物的吸附能力. 实验证明, 在800°C下制备的PNMC组装的硫** 极(S/PNMC-800)表现出优异的电化学性能, 在1 C下经过300圈循环后 仍有556.7 mA h g−1放电比容量. 本工作提出了一种调控碳材料中吡啶 氮含量的简便方法, 为用于锂硫电池的多功能硫载体材料的开发提供 启发.

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Acknowledgements

This work was supported by the National Key R&D Program of China (2021YFB2401800), the National Natural Science Foundation of China (2217090605 and 21875022), and the Natural Science Foundation of Chongqing, China (cstc2020jcyj-msxmX0654 and cstc2020jcyj-msxmX0589). Chen L and Li N acknowledge the support from Bei**g Institute of Technology Research Fund Program for Young Scholars.

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Authors and Affiliations

  1. Bei**g Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Bei**g Institute of Technology, Bei**g, 100081, China

    Lai Chen  (陈来), Chenying Zhao  (赵晨颖), Shuangyi Zhao  (赵双义), Zhiyu Liu  (刘祉妤), Yun Lu  (卢赟), Youxiang Bai  (白友祥), Ning Li  (**宁), Duanyun Cao  (曹端云), Shi Chen  (陈实), Yuefeng Su  (苏岳锋) & Feng Wu  (吴锋)

  2. Bei**g Institute of Technology Chongqing Innovation Center, Chongqing, 401120, China

    Lai Chen  (陈来), Chenying Zhao  (赵晨颖), Zhiyu Liu  (刘祉妤), Yun Lu  (卢赟), Youxiang Bai  (白友祥), Ning Li  (**宁), Duanyun Cao  (曹端云), Yuefeng Su  (苏岳锋) & Feng Wu  (吴锋)

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  1. Lai Chen  (陈来)
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  2. Chenying Zhao  (赵晨颖)
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  3. Shuangyi Zhao  (赵双义)
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  9. Shi Chen  (陈实)
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  10. Yuefeng Su  (苏岳锋)
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Contributions

Wu F proposed the research direction. Chen L, Lu Y, and Su Y conceived and designed the idea. Lu Y guided the research. Zhao C and Zhao S performed the experiments and carried out some data analysis. Liu Z and Bai Y reviewed the manuscript and checked the data. Cao D performed the theoretical calculations. Chen L and Zhao C wrote the manuscript with support from Lu Y. Li N and Chen S proposed some valuable suggestions. All authors participated in the general discussion.

Corresponding authors

Correspondence to Yun Lu  (卢赟) or Yuefeng Su  (苏岳锋).

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Conflict of interest

The authors declare that they have no conflict of interest.

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Supporting data are available in the online version of the paper.

Lai Chen obtained his PhD degree in environmental engineering from Bei**g Institute of Technology (BIT) in 2017 and is currently an associate professor at the school of Materials Science and Engineering, BIT. His research focuses on high-energy-density lithium-ion secondary batteries and their associated materials.

Yun Lu is currently an instructor at the School of Materials Science & Engineering, BIT. She received her BE degree in polymer materials from BIT in 2001, and PhD degree in materials science and engineering from BIT in 2006. Her research includes polymer-based electrolytes for Li-S battery and aerogels of conductive polymers.

Yuefeng Su is a professor at the School of Materials Science and Engineering, BIT. His research group mainly focuses on green secondary batteries and advanced energy materials, including lithium-rich cathode materials, nickel-rich cathode materials and other high-power energy storage devices.

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Facilitating polysulfide confinement using N-doped honeycomb-like carbon with high pyridinic-nitrogen content for high-performance Li-S batteries

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Chen, L., Zhao, C., Zhao, S. et al. Facilitating polysulfide confinement using N-doped honeycomb-like carbon with high pyridinic-nitrogen content for high-performance Li-S batteries. Sci. China Mater. 66, 2169–2180 (2023). https://doi.org/10.1007/s40843-022-2387-1

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