Synchronously Consolidating Li, Se, S, and C for Robust Li-SeS Batteries

Mengmeng Qian, Feng Wu*, Junfan Zhang, Yun Li, Chongteng Wu, Duanyun Cao, Jing Wang, Tinglu Song, Longlong Fan, Yifei Yuan, Jia Qi Huang, Guoqiang Tan*

*Corresponding author for this work

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Abstract

S-redox involving solvated polysulfides is accompanied by volumetric change and structural decay of the S-based cathodes. Here, we propose a synchronous construction strategy for consolidating Li, Se, S, and C elements within a composite cathode via a paradigm reaction of 8Li+2Se+CS2 = 2Li4SeS+C. The obtained composite features crystalline Li4SeS encapsulated in a carbon nanocage (Li4SeS@C), exhibiting ultrahigh electrical conductivity, ultralow activation barrier, and excellent structural integrity, accordingly enabling large specific capacity (615 mAh g-1) and high capacity retention (87.3% after 350 cycles) at 10 A g-1. TOF-SIMS demonstrates its superior volumetric efficiency to a similar derivative SeS@C (2Se+CS2 = 2SeS+C), and DFT reveals its lower activation barrier than Li2S@C and Li2Se@C. This consolidation design significantly improves the electrochemical performance of S-based cathodes, and the paradigm reaction guarantees structural diversity and flexibility. Moreover, employing a synchronous construction mechanism to maximize the synergistic effect between element consolidation and carbon encapsulation opens up a new approach for developing robust S or chalcogenide cathodes.

Original languageEnglish
Pages (from-to)12027-12035
Number of pages9
JournalNano Letters
Volume24
Issue number39
DOIs
Publication statusPublished - 2 Oct 2024

Keywords

  • Li−SeS battery
  • carbon encapsulation
  • element substitution
  • sulfur cathode
  • synchronous consolidation

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Qian, M., Wu, F., Zhang, J., Li, Y., Wu, C., Cao, D., Wang, J., Song, T., Fan, L., Yuan, Y., Huang, J. Q., & Tan, G. (2024). Synchronously Consolidating Li, Se, S, and C for Robust Li-SeS Batteries. Nano Letters, 24(39), 12027-12035. https://doi.org/10.1021/acs.nanolett.4c01388