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Oxygen defects boost polysulfides immobilization and catalytic conversion: First-principles computational characterization and experimental design

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Abstract

Although some experiments have shown that point defects in a cathode host material may enhance its performance for lithium-sulfur battery (LSB), the enhancement mechanism needs to be well investigated for the design of desired sulfur host. Herein, the first principle density functional theory (DFT) is adopted to investigate a high-performance sulfur host material based on oxygen-defective TiO2 (D-TiO2). The adsorption energy comparisons and Gibbs free energy analyses verify that D-TiO2 has relatively better performances than defect-free TiO2 in terms of anchoring effect and catalytic conversion of polysulfides. Meanwhile, D-TiO2 is capable of absorbing the most soluble and diffusive long-chain polysulfides. The newly designed D-TiO2 composited with three-dimensional graphene aerogel (D-TiO2@Gr) has been shown to be an excellent sulfur host, maintaining a specific discharge capacity of 1,049.3 mAhg−1 after 100 cycles at 1C with a sulfur loading of 3.2 mgcm−2. Even with the sulfur mass loading increasing to 13.7 mgcm−2, an impressive stable cycling is obtained with an initial areal capacity of 14.6 mAhcm−2, confirming the effective enhancement of electrochemical performance by the oxygen defects. The DFT calculations shed lights on the enhancement mechanism of the oxygen defects and provide some guidance for designing advanced sulfur host materials.

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Acknowledgements

This work was supported by the Excellent Dissertation Cultivation Funds of Wuhan University of Technology (No. 2018-YS-013).

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Authors and Affiliations

  1. State Key Laboratory of Silicate Materials for Architectures, International School of Materials Science and Engineering, Wuhan University of Technology, Wuhan, 430070, China

    Qiu He, Bin Yu, Huan Wang, Xiaobin Liao & Yan Zhao

  2. Materials Engineering, School of Mechanical and Mining Engineering, The University of Queensland, St Lucia, QLD, 4072, Australia

    Masud Rana

  3. The Institute of Technological Sciences, Wuhan University, Wuhan, 430072, China

    Yan Zhao

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  1. Qiu He
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  2. Bin Yu
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  3. Huan Wang
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  4. Masud Rana
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  5. Xiaobin Liao
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Correspondence to Yan Zhao.

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Oxygen defects boost polysulfides immobilization and catalytic conversion: First-principles computational characterization and experimental design

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He, Q., Yu, B., Wang, H. et al. Oxygen defects boost polysulfides immobilization and catalytic conversion: First-principles computational characterization and experimental design. Nano Res. 13, 2299–2307 (2020). https://doi.org/10.1007/s12274-020-2850-5

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