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Nano Research 2016, 9(1): 240-248 https://doi.org/10.1007/s12274-016-1005-1
Research Article | Issue | Published: 29 January 2016

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

Show Author's Information Benjamin Papandrea1,§,  Xu Xu1,2,§,  Yuxi Xu1,  Chih-Yen Chen3,  Zhaoyang Lin1,  Gongming Wang1,  Yanzhu Luo2,  Matthew Liu3,  Yu Huang3,4,  Liqiang Mai2( ),  Xiangfeng Duan1,4( )
Department of Chemistry and BiochemistryUniversity of CaliforniaLos AngelesCA90095USA
State Key Laboratory of Advanced Technology for Materials Synthesis and ProcessingWuhan University of TechnologyWuhan430070China
Department of Materials Science and EngineeringUniversity of CaliforniaLos AngelesCA90095USA
California NanoSystems InstituteUniversity of CaliforniaLos AngelesCA90095USA

§ These authors contributed equally to this work.

Keywords:
energy storage, graphene framework, three-dimensional (3D)-network, high loading, lithium sulfur battery
Cite this article:
Papandrea B, Xu X, Xu Y, et al. Three-dimensional graphene framework with ultra-high sulfur content for a robust lithium–sulfur battery. Nano Research, 2016, 9(1): 240-248. https://doi.org/10.1007/s12274-016-1005-1
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Abstract Full text Electronic supplementary material About this article

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 96 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.


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Electronic supplementary material
About this article

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

Show Author's information Benjamin Papandrea1,§, Xu Xu1,2,§, Yuxi Xu1, Chih-Yen Chen3, Zhaoyang Lin1, Gongming Wang1, Yanzhu Luo2, Matthew Liu3, Yu Huang3,4, Liqiang Mai2( ), Xiangfeng Duan1,4( )
Department of Chemistry and BiochemistryUniversity of CaliforniaLos AngelesCA90095USA
State Key Laboratory of Advanced Technology for Materials Synthesis and ProcessingWuhan University of TechnologyWuhan430070China
Department of Materials Science and EngineeringUniversity of CaliforniaLos AngelesCA90095USA
California NanoSystems InstituteUniversity of CaliforniaLos AngelesCA90095USA

§ These authors contributed equally to this work.

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 96 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.

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

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Publication history
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Acknowledgements

Publication history

Received: 18 December 2015
Accepted: 05 January 2016
Published: 29 January 2016
Issue date: January 2016

Copyright

© Tsinghua University Press and Springer-Verlag Berlin Heidelberg 2016

Acknowledgements

Acknowledgements

We acknowledge the Electron Imaging Center for Nanomachines (EICN) at the California NanoSystems Institute for the technical support of TEM. X. F. D. acknowledges partial support by a Dupont Young Professor Award. X. X. would like to acknowledge the Chinese Scholarship Council (CSC) for financial support.

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