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Nano Research

Article Title

Three-dimensionally ordered, ultrathin graphitic-carbon frameworks with cage-like mesoporosity for highly stable Li-S batteries

Authors

Huijuan Yu, 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
Hanwen Li, 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
Shouyi Yuan, 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
Yuchi Yang, 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
Jiahui Zheng, 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
Jianhua Hu, State Key Laboratory of Molecular Engineering of Polymers and Department of Macromolecular Science, Fudan University, Shanghai 200433, China
Dong Yang, State Key Laboratory of Molecular Engineering of Polymers and Department of Macromolecular Science, Fudan University, Shanghai 200433, China
Yonggang Wang, 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
Angang Dong, 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

Keywords

self-assembly, nanoparticles, graphene frameworks, cage-like mesoporosity, Li-S batteries

Abstract

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.

Graphical Abstract

Publisher

Tsinghua University Press

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