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Three-dimensionally ordered,ultrathin graphitic-carbon frameworks with cage-like mesoporosity for highly stable Li-S batteries
Authors:Yu  Huijuan  Li  Hanwen  Yuan  Shouyi  Yang  Yuchi  Zheng  Jiahui  Hu  Jianhua  Yang  Dong  Wang  Yonggang  Dong  Angang
Affiliation:1. Collaborative Innovation Center of Chemistry for Energy Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, and Department of Chemistry, Fudan University, Shanghai 200433, China;State Key Laboratory of Molecular Engineering of Polymers and Department of Macromolecular Science, Fudan University, Shanghai 200433, China;2. Collaborative Innovation Center of Chemistry for Energy Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, and Department of Chemistry, Fudan University, Shanghai 200433, China;3. State Key Laboratory of Molecular Engineering of Polymers and Department of Macromolecular Science, Fudan University, Shanghai 200433, China
Abstract:Mesoporous carbons have been widely utilized as the sulfur host for lithium-sulfur (Li-S) batteries.The ability to engineer the porosity,wall thickness,and graphitization degree of the carbon host is essential for addressing issues that hamper commercialization of Li-S batteries,such as fast capacity decay and poor high-rate performance.In this work,highly ordered,ultrathin mesoporous graphitic-carbon frameworks (MGFs) having unique cage-like mesoporosity,derived from self-assembled Fe3O4 nanoparticle superlattices,are demonstrated to be an excellent host for encapsulating sulfur.The resulting S@MGFs exhibit high specific capacity (1,446 mAh·g-1 at 0.15 C),good rate capability (430 mAh.g-1 at 6 C),and exceptional cycling stability (~0.049% capacity decay per cycle at 1 C) when used as Li-S cathodes.The superior electrochemical performance of the S@MGFs is attributed to the many unique and advantageous structural features of MGFs.In addition to the interconnected,ultrathin graphitic-carbon framework that ensures rapid electron and lithium-ion transport,the microporous openings between adjacent mesopores efficiently suppress the diffusion of polysulfides,leading to improved capacity retention even at high current densities.
Keywords:self-assembly  nanoparticles  graphene frameworks  cage-like mesoporosity  Li-S batteries
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