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Nitrogen-doped microporous carbon with narrow pore size distribution as sulfur host to encapsulate small sulfur molecules for highly stable lithium-sulfur batteries

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Abstract

Lithium-sulfur (Li-S) battery with high theoretical energy density has been considered as an important energy storage system. However, its application has been limited by low cycling stability and rapid capacity decay due to the shuttle of lithium polysulfide (Li2Sn, n > 5). These problems can be solved using small sulfur molecules (S2–4) as the active material, while synthesis of carbon hosts with suitable pores size and narrow pore distribution to encapsulate small sulfur molecules are still challenging. Here, we report a novel nitrogen-doping microporous carbon (NDMC) sulfur host with narrow micropore unimodal size distribution centered at 0.57 nm. By accommodating small sulfur molecules (S2–4) within the subnanopores of NDMC, the formation and shuttle of soluble lithium polysulfide (LiPS) can be avoided. The cathode shows only a long potential plateau due to the direct conversion from S2–4 to Li2S. In carbonate-based electrolyte, the NDMC/S-2 cathode remains a stable and reversible capacity of 902 mAh g−1 at 0.2 C with 100% Coulombic efficiency after 500 cycles, and capacity fading per cycle is only around 0.02%. Besides, an excellent capacity of 511.8 mAh g−1 is achieved even at an ultrahigh rate of 10 C, demonstrating a superior rate capability performance. This NDMC/S composite also shows excellent cycling stability in ether-based electrolyte. All the above demonstrate the NDMC has great potential application in Li-S batteries.

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Funding

This work was financially supported by the National Natural Science Foundation of China (Grant Nos. 51772089, 52072118, and 21872046), the Outstanding Youth Scientist Foundation of Hunan Province (Grant No. 2018JJ1009), the Youth 1000 Talent Program of China, the Science and Technology Innovation Platform and Talent Plan of Hunan Province (Grant No. 2017XK2023), the Natural Science Foundation of Hunan Province, the Research and Development Plan of Key Areas in Hunan Province (Grant No. 2019GK2235), and the Key Research and Development Program of Ningxia (2020BDE03007).

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Authors and Affiliations

  1. College of Materials Science and Engineering, Hunan University, Changsha, 410082, China

    Mingnan Li, Zhaoen Liu, Yan Zhang, Xiwen Wang & Shiguo Zhang

  2. Nanophotonics and Optoelectronics Research Center, Qian Xuesen Laboratory of Space Technology, China Academy of Space Technology, Beijing, 100094, China

    Ce Zhang

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  1. Mingnan Li
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  2. Zhaoen Liu
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  3. Yan Zhang
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  4. Xiwen Wang
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  5. Ce Zhang
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Correspondence to Xiwen Wang, Ce Zhang or Shiguo Zhang.

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Li, M., Liu, Z., Zhang, Y. et al. Nitrogen-doped microporous carbon with narrow pore size distribution as sulfur host to encapsulate small sulfur molecules for highly stable lithium-sulfur batteries. J Solid State Electrochem 25, 1293–1302 (2021). https://doi.org/10.1007/s10008-021-04907-z

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