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In-situ UV-Vis Spectroscopy of Trisulfur Radicals in Lithium-Sulfur Batteries

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Abstract

Here we employ in-situ UV-Vis spectroscopy to monitor the sulfur redox reaction with oxygen-containing molecules as an additive, for example, biphenyl-4,4′-dicarboxylic acid (BDC). Furthermore, Raman spectrum, electron paramagnetic resonance (EPR), and electrospray ionization-mass spectrometry (ESI-MS) measurements reveal that the formation of BDC-S •‒3 complexes can establish the long-term stability of polysulfide radicals, change the kinetics of sulfur redox reaction, and then generate decent capacity retention and rate capability. According to the density functional theory (DFT) analysis, S •‒3 radicals are the underlying product of S 2‒6 cleavage, owing to the decreased chemical energy and the increased stability of S •‒3 radicals through Lewis acid-base interaction. The assembled Li-S batteries with BDC additive deliver a high reversible capacity of 420 mA·h·g−1 over 200 cycles with over 98% Coulombic efficiency, under the current density of 0.2 C.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 21874127, 21721003) and the Development Program of Jilin Province of China (No. YDZJ202101ZYTS164).

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Authors and Affiliations

  1. School of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei, 230026, P. R. China

    Renju Dou, Qin Wang, Xiaoyan Ren & Lehui Lu

  2. State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, 130022, P. R. China

    Renju Dou, Qin Wang, Xiaoyan Ren & Lehui Lu

Authors
  1. Renju Dou
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  2. Qin Wang
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  3. Xiaoyan Ren
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  4. Lehui Lu
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Corresponding authors

Correspondence to Xiaoyan Ren or Lehui Lu.

Ethics declarations

LU Lehui is an editorial board member for Chemical Research in Chinese Universities and was not involved in the editorial review or the decision to publish this article. The authors declare no conflicts of interest.

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Dou, R., Wang, Q., Ren, X. et al. In-situ UV-Vis Spectroscopy of Trisulfur Radicals in Lithium-Sulfur Batteries. Chem. Res. Chin. Univ. 40, 279–286 (2024). https://doi.org/10.1007/s40242-024-4027-3

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  • DOI: https://doi.org/10.1007/s40242-024-4027-3

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