Chemical Research in Chinese Universities ›› 2024, Vol. 40 ›› Issue (4): 690-698.doi: 10.1007/s40242-024-4155-9

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Balanced Polysulfide Containment and Lithium Ion Transport in Lithium-Sulfur Batteries via Nitrogen-doped Carbon Hollow Multi-shelled Structures on Modified Separators

RAO Fu1,4, XIAO Qian1,3, WEI Yanze1,2, WANG Jiangyan1,2,3, YU Ranbo4, WANG Dan1,2,3   

  1. 1. State Key Laboratory of Biochemical Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, P. R. China;
    2. Key Laboratory of Biopharmaceutical Preparation and Delivery, Chinese Academy of Sciences, Beijing 100190, P. R. China;
    3. University of Chinese Academy of Sciences, Beijing 100049, P. R. China;
    4. Department of Physical Chemistry, School of Metallurgical and Ecological Engineering, University of Science & Technology Beijing, Beijing 100083, P. R. China
  • Received:2024-07-04 Online:2024-08-01 Published:2024-07-24
  • Contact: WEI Yanze,yzwei@ipe.ac.cn;YU Ranbo,ranboyu@ustb.edu.cn;WANG Dan,danwang@ipe.ac.cn E-mail:yzwei@ipe.ac.cn;ranboyu@ustb.edu.cn;danwang@ipe.ac.cn
  • Supported by:
    This work was supported by the National Natural Science Foundation of China (Nos. 21821005, 21931012, 21820102002, 22293043, 52272097, 52372170), the Beijing Natural Science Foundation, China (No. 2242019) and the DNL Cooperation Fund, Chinese Academy of Sciences (CAS) (No. DNL202020).

Abstract: Representing the next-generation technology in lithium-ion batteries, lithium-sulfur (Li-S) batteries offer increased specific energy without relying on scarce metals like nickel and cobalt, but suffer from a low practical specific energy due to poor conductivity and a short lifespan due to the shuttle effect of polysulfides. Balancing the confinement of polysulfides and the transport of lithium ions requires highly elaborate modifiers for separators. Hollow multi-shelled structures (HoMS) show promise as hierarchical mesostructures for separators, offering multiple shell layers and internal cavities that effectively inhibit polysulfide shuttle. Thoughtful design of these structures is crucial to address these challenges effectively. In this study, nitrogen-doped carbon HoMS (NC HoMS) was created using polymer templates through a precisely controlled polymerization process. Batteries featuring NC HoMS-modified separators exhibit improved capacity and cycling stability in comparison to those utilizing commercial separators. Especially, triple-shelled NC HoMS strikes a balance in polysulfide containment and lithium ion transport. Featuring a sulfur loading of 6.34 mg/cm2, the Li-S battery can consistently complete 100 charge-discharge cycles, starting with a discharge capacity of 966.4 mA∙h/g with a 75.8% capacity retention rate. NC HoMS holds potential as the separator modifier in addressing the polysulfide shuttle problem and facilitating the Li-ion transportation for advanced Li-S batteries.

Key words: Hollow multi-shelled structure, Carbon material, Li-S battery, Separator modification, Shuttle effect