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Nano Research 2022, 15(9): 7925-7932 https://doi.org/10.1007/s12274-022-4453-9
Research Article | Issue | Published: 08 June 2022

Quantitative defect regulation of heterostructures for sulfur catalysis toward fast and long lifespan lithium-sulfur batteries

Show Author's Information Saisai Qiu1,§,  Xinqi Liang1,§,  Shuwen Niu2,  Qingguo Chen1,  Gongming Wang2( ),  Minghua Chen1( )
Key Laboratory of Engineering Dielectric and Applications (Ministry of Education), School of Electrical and Electronic Engineering, Harbin University of Science and Technology, Harbin 150080, China
Hefei National Laboratory for Physical Science at the Microscale, Department of Chemistry, University of Science & Technology of China, Hefei 230026, China

§ Saisai Qiu and Xinqi Liang contributed equally to this work.

Keywords:
shuttle effect, lithium polysulfides (LiPSs), lithium-sulfur (Li-S) batteries, redox kinetics, selenium vacancy, sulfur catalysis
Topics:
Catalysis
Cite this article:
Qiu S, Liang X, Niu S, et al. Quantitative defect regulation of heterostructures for sulfur catalysis toward fast and long lifespan lithium-sulfur batteries. Nano Research, 2022, 15(9): 7925-7932. https://doi.org/10.1007/s12274-022-4453-9
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Abstract Full text Electronic supplementary material About this article

The advancement of lithium-sulfur (Li-S) batteries is severely retarded by lithium polysulfides (LiPSs) shuttling behavior and sluggish redox kinetics. Herein, the heterogeneous composite with defective Bi2Se3−x nanosheets and porous nitrogen-doped carbon (Bi2Se3−x/NC) is prepared by selenizing bismuth metal-organic frameworks as a multifunctional sulfur host. The highly efficient immobilization-conversion on LiPSs is realized by the synergistic effect of structure construction strategy and defect engineering. It is found that Bi2Se3−x with the suitable amount of selenium vacancies achieves the best electrochemical performance due to the advantages of its structure and composition. These results confirm the intrinsic correlation between defects and catalysis, which are revealed by computational and experimental studies. Due to these superiorities, the developed sulfur electrodes exhibited admirable stability and a fairly lower capacity decay rate of approximately 0.0278% per cycle over 1,000 cycles at a 3 C rate. Even at the high sulfur loading of 6.2 mg·cm−2, the cathode still demonstrates a high discharge capacity of 455 mAh·g−1 at 1 C. This work may enlighten the development of mechanism investigation and design principles regarding sulfur catalysis toward high-performance Li-S batteries.


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Electronic supplementary material
About this article

Quantitative defect regulation of heterostructures for sulfur catalysis toward fast and long lifespan lithium-sulfur batteries

Show Author's information Saisai Qiu1,§, Xinqi Liang1,§, Shuwen Niu2, Qingguo Chen1, Gongming Wang2( ), Minghua Chen1( )
Key Laboratory of Engineering Dielectric and Applications (Ministry of Education), School of Electrical and Electronic Engineering, Harbin University of Science and Technology, Harbin 150080, China
Hefei National Laboratory for Physical Science at the Microscale, Department of Chemistry, University of Science & Technology of China, Hefei 230026, China

§ Saisai Qiu and Xinqi Liang contributed equally to this work.

Abstract

The advancement of lithium-sulfur (Li-S) batteries is severely retarded by lithium polysulfides (LiPSs) shuttling behavior and sluggish redox kinetics. Herein, the heterogeneous composite with defective Bi2Se3−x nanosheets and porous nitrogen-doped carbon (Bi2Se3−x/NC) is prepared by selenizing bismuth metal-organic frameworks as a multifunctional sulfur host. The highly efficient immobilization-conversion on LiPSs is realized by the synergistic effect of structure construction strategy and defect engineering. It is found that Bi2Se3−x with the suitable amount of selenium vacancies achieves the best electrochemical performance due to the advantages of its structure and composition. These results confirm the intrinsic correlation between defects and catalysis, which are revealed by computational and experimental studies. Due to these superiorities, the developed sulfur electrodes exhibited admirable stability and a fairly lower capacity decay rate of approximately 0.0278% per cycle over 1,000 cycles at a 3 C rate. Even at the high sulfur loading of 6.2 mg·cm−2, the cathode still demonstrates a high discharge capacity of 455 mAh·g−1 at 1 C. This work may enlighten the development of mechanism investigation and design principles regarding sulfur catalysis toward high-performance Li-S batteries.

Keywords: shuttle effect, lithium polysulfides (LiPSs), lithium-sulfur (Li-S) batteries, redox kinetics, selenium vacancy, sulfur catalysis

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Publication history
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Acknowledgements

Publication history

Received: 07 March 2022
Revised: 28 March 2022
Accepted: 20 April 2022
Published: 08 June 2022
Issue date: September 2022

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (No. 52122702), the Natural Science Foundation of Heilongjiang Province of China (No. JQ2021E005), and the Fundamental Research Foundation for Universities of Heilongjiang Province (No. LGYC2018JQ006).

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