Enlarged interlayer of separator coating enabling high-performance lithiumsulfur batteries

Abstract

Lithiumsulfur batteries have been intensively studied due to their high theoretical energy density and abundant sulfur resources. However, their commercial application is hindered by the low redox kinetics and high sulfur losses. In principle, in the design of cathodes and separators, the adsorption toward lithium-polysulfides should be enhanced and the conversion of soluble high-order lithium-polysulfides should be catalyzed. Herein, a KV₃O₈·0.75H₂O separator is designed as an effective lithium-polysulfides mediator in lithiumsulfur batteries. The intercalated K⁺ would enlarge the interlayer spacing of vanadium oxides, preventing the collapse of the layer structure and improving the electrical/ion conductivity of the interface. Moreover, the KV₃O₈·0.75H₂O modified separator possess a prior adsorption and high redox kinetics toward lithium-polysulfides due to the enhanced diffusion kinetics, which guarantees the high-rate capability and efficient utilization of sulfur. As a result, lithiumsulfur batteries exhibit a high capacity of 1362 mAh·g¹ and a long lifespan with a low capacity loss of 0.073% per cycle. This work may provide an alternative way to establish a functional separator to balance the adsorption and conversion of polysulfides during the redox back and forth.

Competing interests

The authors declare that they have no competing interests.

Acknowledgements

Lu Q would like to acknowledge the financial supports from Joint Fund of Henan Province Science and Technology R&D Program (Grant No. 225200810093) and Startup Research of Henan Academy of Sciences (Grant No. 231817001). We also acknowledge financial supports from the National Natural Science Foundation of China (Grant No. 51272147), the Natural Science Foundation of Shaanxi Province (Grant No. 2015JM5208), the Graduate Innovation Found of Shaanxi University of Science and Technology, and Scientific Research Project of Chengdu Technological University (Grant No. 2023RC001). This work is also supported by the National Key R&D Program of China (Grant No. 2019YFC1520100). Feng Y acknowledge the financial supports from China Scholarship Council. The authors thank Andrea Voß (IFW Dresden) for technical support and ICP test. Beamtime allocation and support at beamline P65 of the PETRA III synchrotron (Deutsches Elektronen-Synchrotron, DESY, Hamburg, Germany) is gratefully acknowledged. Daria Mikhailova (IFW Dresden) is acknowledged for XAS measurement.

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11705-024-2385-5 and is accessible for authorized users.

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