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Restraining the shuttle effects of lithium polysulfides is the key to improve the cycling reversibility and stability of lithium-sulfur (Li-S) batteries for which design of robust sulfur hosts has been regarded as the most effective strategy. In this work, we report a new type of hybrid sulfur host which is composed of Al2O3 homogenously decorated in nitrogen-rich mesoporous carbon framework (NMC-Al2O3). The NMC-Al2O3 hybrid host features a poly-dispersed spherical morphology and a mesoporous configuration with high surface area and large pore volume that can accommodate a high sulfur content up to 73.5 wt.%. As a result, the fabricated NMC-Al2O3-S cathode exhibits all-round improvements in electrochemical properties in term of capacities (1,212 mAh·g-1 at 0.2 C; 755 mAh·g-1 at 2 C), cycling charge-discharge reversibility (sustainably 100% efficiencies) and stability (1,000 cycles with only 0.023% capacity decay per cycle at 0.5 C). By contrast, the Al2O3-free NMC-S cathode shows both decreased capacities and rapidly descending Coulombic efficiencies during cycling. Density functional theory (DFT) calculations further reveal that the implanted Al2O3 can greatly enhance the chemical adsorption and catalytic conversion for various lithium polysulfides and thereby effectively prevent the polysulfide shuttling and significantly improve the utilizability, reversibility and stability of sulfur cathode.


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Vapor deposition of aluminium oxide into N-rich mesoporous carbon framework as a reversible sulfur host for lithium-sulfur battery cathode

Show Author's information Fei Sun1( )Zhibin Qu1Hua Wang1Xiaoyan Liu2Tong Pei1Rui Han1Jihui Gao1Guangbo Zhao1Yunfeng Lu3( )
School of Energy Science and Engineering, Harbin Institute of Technology, Harbin 150001, China
Department of Chemistry, Shanghai Normal University, Shanghai 150001, China
Department of Chemical and Biomolecular Engineering, University of California, Los Angeles, CA 90095, USA

Abstract

Restraining the shuttle effects of lithium polysulfides is the key to improve the cycling reversibility and stability of lithium-sulfur (Li-S) batteries for which design of robust sulfur hosts has been regarded as the most effective strategy. In this work, we report a new type of hybrid sulfur host which is composed of Al2O3 homogenously decorated in nitrogen-rich mesoporous carbon framework (NMC-Al2O3). The NMC-Al2O3 hybrid host features a poly-dispersed spherical morphology and a mesoporous configuration with high surface area and large pore volume that can accommodate a high sulfur content up to 73.5 wt.%. As a result, the fabricated NMC-Al2O3-S cathode exhibits all-round improvements in electrochemical properties in term of capacities (1,212 mAh·g-1 at 0.2 C; 755 mAh·g-1 at 2 C), cycling charge-discharge reversibility (sustainably 100% efficiencies) and stability (1,000 cycles with only 0.023% capacity decay per cycle at 0.5 C). By contrast, the Al2O3-free NMC-S cathode shows both decreased capacities and rapidly descending Coulombic efficiencies during cycling. Density functional theory (DFT) calculations further reveal that the implanted Al2O3 can greatly enhance the chemical adsorption and catalytic conversion for various lithium polysulfides and thereby effectively prevent the polysulfide shuttling and significantly improve the utilizability, reversibility and stability of sulfur cathode.

Keywords: mesoporous structure, lithium-sulfur battery, sulfur host, aluminium oxide, nitrogen-rich carbon

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Publication history
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Acknowledgements

Publication history

Received: 29 July 2020
Revised: 12 August 2020
Accepted: 13 August 2020
Published: 05 January 2021
Issue date: January 2021

Copyright

© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature

Acknowledgements

This work is supported by the Open Project of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering, Ningxia University (No. 2018-13K) and the Fundamental Research Funds for the Central Universities.

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