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Sulfurized polyacrylonitrile (SPAN) cathode exhibits improved cycling stability in carbonate electrolytes due to the existent of –Sx2−– (2 ≤ n ≤ 4) units. However, it is still challenging for SPAN to achieve higher sulfur content, superior conductivity, and faster polysulfide conversion kinetics in ether electrolytes. Herein, polyacrylonitrile (PAN), 2-morpholinothiobenzothiazole (MBS), and FeCl3 coated reduced graphene oxide (rGO) were used to fabricate advanced sulfur cathode through electrospinning technology to address these problems. During PAN sulfuration reactions, the MBS with abundant unsaturated bonds served as the vulcanization accelerator to facilitate the formation of longer chain sulfur species (–S3–/–S4–) and increase the sulfur content in the SPAN electrode system. Meanwhile, Fe1−xS is in situ converted from FeCl3, which acts as the electrocatalyst to promote Li2S nucleation and decomposition reactions. As a result, the Fe1−xS/SPAN/rGO electrode with high sulfur loading of 2.0 mg·cm−2 delivers a reversible capacity of 1122 mAh·g−1 at 0.1 A·g−1. Notably, at a large current density of 5.0 A·g−1, the Fe1−xS/SPAN/rGO electrode still displays a high specific capacity of 924 mAh·g−1 with an ultra-stable cycling life over 2000 cycles. The present work provides new insights into designing of high-performance electrode materials for long-lasting Li-S batteries.


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Sulfurization accelerator coupled Fe1−xS electrocatalyst boosting SPAN cathode performance

Show Author's information Jinlei Qin,§Yun Lu,§Rui WangZhizhan LiTao ShenDeli Wang( )
Key Laboratory of Materials Chemistry for Energy Conversion and Storage of Ministry of Education, Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan 430074, China

§ Jinlei Qin and Yun Lu contributed equally to this work.

Abstract

Sulfurized polyacrylonitrile (SPAN) cathode exhibits improved cycling stability in carbonate electrolytes due to the existent of –Sx2−– (2 ≤ n ≤ 4) units. However, it is still challenging for SPAN to achieve higher sulfur content, superior conductivity, and faster polysulfide conversion kinetics in ether electrolytes. Herein, polyacrylonitrile (PAN), 2-morpholinothiobenzothiazole (MBS), and FeCl3 coated reduced graphene oxide (rGO) were used to fabricate advanced sulfur cathode through electrospinning technology to address these problems. During PAN sulfuration reactions, the MBS with abundant unsaturated bonds served as the vulcanization accelerator to facilitate the formation of longer chain sulfur species (–S3–/–S4–) and increase the sulfur content in the SPAN electrode system. Meanwhile, Fe1−xS is in situ converted from FeCl3, which acts as the electrocatalyst to promote Li2S nucleation and decomposition reactions. As a result, the Fe1−xS/SPAN/rGO electrode with high sulfur loading of 2.0 mg·cm−2 delivers a reversible capacity of 1122 mAh·g−1 at 0.1 A·g−1. Notably, at a large current density of 5.0 A·g−1, the Fe1−xS/SPAN/rGO electrode still displays a high specific capacity of 924 mAh·g−1 with an ultra-stable cycling life over 2000 cycles. The present work provides new insights into designing of high-performance electrode materials for long-lasting Li-S batteries.

Keywords: Li-S batteries, electrocatalyst, electrospun, vulcanization accelerators, sulfurized polyacrylonitrile (SPAN)

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Publication history
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Publication history

Received: 28 November 2022
Revised: 13 February 2023
Accepted: 13 February 2023
Published: 26 June 2023
Issue date: July 2023

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© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This work was supported by the National Key R&D Program of China (No. 2018YFB0905600) and the Innovation Research Funds of Huazhong University of Science and Technology (HUST, No. 2172019kfyRCPY100). The authors thank the Analytical and Testing Center of HUST for allowing the use of its facilities.

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