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Nano Research

Article Title

Three-dimensional graphene framework with ultra-high sulfur content for a robust lithium–sulfur battery

Authors

Benjamin Papandrea, Department of Chemistry and Biochemistry, University of California, Los Angeles, CA 90095, USA
Xu Xu, Department of Chemistry and Biochemistry, University of California, Los Angeles, CA 90095, USA State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China
Yuxi Xu, Department of Chemistry and Biochemistry, University of California, Los Angeles, CA 90095, USA
Chih-Yen Chen, Department of Materials Science and Engineering, University of California, Los Angeles, CA 90095, USA
Zhaoyang Lin, Department of Chemistry and Biochemistry, University of California, Los Angeles, CA 90095, USA
Gongming Wang, Department of Chemistry and Biochemistry, University of California, Los Angeles, CA 90095, USA
Yanzhu Luo, State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China
Matthew Liu, Department of Materials Science and Engineering, University of California, Los Angeles, CA 90095, USA
Yu Huang, Department of Materials Science and Engineering, University of California, Los Angeles, CA 90095, USA California NanoSystems Institute, University of California, Los Angeles, CA 90095, USA
Liqiang Mai, State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China
Xiangfeng Duan, Department of Chemistry and Biochemistry, University of California, Los Angeles, CA 90095, USA California NanoSystems Institute, University of California, Los Angeles, CA 90095, USA

Keywords

energy storage, graphene framework, three-dimensional (3D)-network, high loading, lithium sulfur battery

Abstract

Lithium–sulfur batteries can deliver significantly higher specific capacity than standard lithium ion batteries, and represent the next generation of energy storage devices for both electric vehicles and mobile devices. However, the lithium–sulfur technology today is plagued with numerous challenges, including poor sulfur conductivity, large volumetric expansion, severe polysulfide shuttling and low sulfur utilization, which prevent its wide-spread adoption in the energy storage industry. Here we report a freestanding three-dimensional (3D) graphene framework for highly efficient loading of sulfur particles and creating a high capacity sulfur cathode. Using a one-pot synthesis method, we show a mechanically robust graphene–sulfur composite can be prepared with the highest sulfur weight content (90% sulfur) reported to date, and can be directly used as the sulfur cathode without additional binders or conductive additives. The graphene–sulfur composite features a highly interconnected graphene network ensuring excellent conductivity and a 3D porous structure allowing efficient ion transport and accommodating large volume expansion. Additionally, the 3D graphene framework can also function as an effective encapsulation layer to retard the polysulfide shuttling effect, thus enabling a highly robust sulfur cathode. Electrochemical studies show that such composite can deliver a highest capacity of 969 mAh·g–1, a record high number achieved for all sulfur cathodes reported to date when normalized by the total mass of the entire electrode. Our studies demonstrate that the 3D graphene framework represents an attractive scaffold material for a high performance lithium sulfur battery cathode, and could enable exciting opportunities for ultra-high capacity energy storage applications.

Graphical Abstract

Publisher

Tsinghua University Press

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