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High-Reaction Kinetics SexS1–x Cathodes for All-Solid-State Lithium–Sulfur Batteries

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Abstract

All-solid-state lithium–sulfur batteries are considered one of the most promising candidates for energy storage devices due to their high energy density and safety. However, the poor electron transport of sulfur-based cathodes significantly reduces their reaction kinetics, resulting in low utilization efficiency and subpar rate performance. Herein, leveraging the similar chemical properties of sulfur and selenium, we uniformly deposit SexS1−x (x = 0–0.3) solid solutions with different selenium content on the surface of active carbon via a facile melt-diffusion method to achieve SexS1−x@AC (x = 0–0.3) composite materials. The introduction of selenium effectively enhances the lithium-ion diffusion coefficient of the SexS1−x@AC (x = 0–0.3) cathodes, and improves the stability of the cathode/solid electrolyte interface. With the increase in selenium content, the reaction kinetics of the SexS1−x@AC (x = 0–0.3) cathodes are altered. Specifically, the average lithium-ion diffusion coefficients for the S@AC and Se0.2S0.8@AC cathodes are 6.11 × 10−14 and 1.65 × 10−13 cm2 s−1, respectively, showing a twofold increase. Concurrently, the Se0.2S0.8@AC cathode exhibits higher discharge capacity (698.8 mA h g−1) than that of the S@AC cathode (501.3 mA h g−1) at 1 A g−1. Surprisingly, even when the mass loading increases to 8.85 mg cm−2, the Se0.2S0.8@AC cathode still shows superior cycling stability, which is attributed to the fast ionic/electronic transport pathways within the cathode. Moreover, the Se0.2S0.8@AC cathode maintains good physical contact at the cathode/SE interface after cycling.

Graphical Abstract

In all-solid-state lithium–sulfur batteries, the introduction of selenium in the sulfur cathode enhances reaction kinetics (1.65 × 10−13 cm2 s−1), provides additional reactive sites, and significantly improves the electrochemical performance of Se0.2S0.8@AC even with high mass loading (8.85 mg cm−2).

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Acknowledgments

The authors gratefully acknowledge financial supports from National Natural Science Foundation of China (22279116 and U20A20253), Natural Science Foundation of Zhejiang Province (LD22E020006 and LQ24E020012), Science and Technology Development of Zhejiang Province (2023C01231 and 2024C01095), the Baima Lake Laboratory Joint Funds of the Zhejiang Provincial Natural Science Foundation (LBMHD24E020001), and China Postdoctoral Science Foundation (2020M671785 and 2020T130597).

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  1. Rui Wu and Ruyi Fang contributed equally to this work.

Authors and Affiliations

  1. College of Materials Science and Engineering, Zhejiang University of Technology, Hangzhou, 310014, China

    Rui Wu, Ruyi Fang, Chengwei Lu, Yong** Gan, ** He, Wenkui Zhang & Yang ** Xu & Zheyu **

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Contributions

RW: Investigation, Data curation, Writing—Original draft. RF: Conceptualization, Funding acquisition, Writing—Original draft. CL: Methodology, Investigation, Data curation. YG: Formal analysis, Visualization. XH: Methodology, Data curation. JX: Investigation, Formal analysis. ZJ: Investigation, Formal analysis. WZ: Investigation, Funding acquisition. YX: Funding acquisition, Writing—Review and editing.

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Correspondence to Ruyi Fang or Yang **a.

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Wu, R., Fang, R., Lu, C. et al. High-Reaction Kinetics SexS1–x Cathodes for All-Solid-State Lithium–Sulfur Batteries. J. Electron. Mater. 53, 2833–2841 (2024). https://doi.org/10.1007/s11664-024-11071-3

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