A Nanocrystallite CuS/Nitrogen-Doped Carbon Host Improves Redox Kinetics in All-Solid-State Li2S Batteries

Yue Yu, Baltej Singh, Zhuo Yu, Chun Yuen Kwok, Ivan Kochetkov, Linda F. Nazar

Research output: Contribution to journalArticlepeer-review

8 Scopus citations

Abstract

All-solid-state Li–S batteries are a promising energy storage system that can solve the shuttle effects of polysulfides in liquid Li–S batteries. However, sluggish solid-state reaction kinetics and the low conductivity of cathode materials have impeded their development. Here, a N-doped carbon embedded with CuS nanoparticles (CuSNC) is reported as a host for Li2S in all-solid-state batteries that addresses some of these issues. Electrochemical studies, supported by a combination of X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), X-ray absorption spectroscopy (XAS), electron microscopy, and density functional theory (DFT) calculations reveal that CuSNC provides good affinity to Li2S. This lowers the activation barrier for the conversion of Li2S to sulfur on the charge, suggesting an electrocatalytic effect on the CuS surface. Li+ diffusion in the cathode and the reaction kinetics are enhanced compared to N-doped graphene. The CuSNC/Li2S cathode reaches an areal capacity of 1.8 mAh cm−2 and a retention rate of 94% after 100 cycles. At a 1.0 mA cm−2 current density, CuSNC/Li2S maintains stable performance over 500 cycles with a low decay rate (0.05% per cycle); at a higher Li2S loading, delivers a capacity of 9.6 mAh cm−2, albeit with more limited cycling. This study provides a promising way to design Li2S cathodes to achieve improved reaction kinetics and better electrochemical performance.

Original languageEnglish
Article number2400845
JournalAdvanced Energy Materials
Volume14
Issue number27
DOIs
StatePublished - Jul 19 2024
Externally publishedYes

Funding

This work was financially supported by Conamix, Inc, and the Ontario Research Fund. The authors graciously thank Dr. Peter Brodersen at the University of Toronto for carrying out the XPS, Mark Wolfman at the Advanced Photon Source (Argonne National Laboratory) for the XANES study, and Dr. Lei Zhang for the TEM study.

Keywords

  • LiS cathode
  • LiS redox
  • Li–sulfur battery
  • all-solid-state batteries
  • argyrodite solid-state electrolyte

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