AI Article Synopsis

  • - Electrocatalysts are crucial in preventing the shuttling effect in lithium-sulfur (Li-S) batteries, but understanding the sulfur redox reactions at the electrocatalyst/LiPS interface is difficult when active sites are obstructed by discharge products.
  • - The study reveals that the LiS (100) plane has intrinsic autocatalytic activity towards lithium polysulfides (LiPS) when used with single-atom nickel (SANi) electrocatalysts, leading to dissociation of LiPS into LiS and short-chain LiPS.
  • - This autocatalytic process generates new LiS (100) surfaces and keeps LiPS concentrations low, allowing Li-S batteries to achieve improved electrochemical performance

Article Abstract

Electrocatalysts are extensively employed to suppress the shuttling effect in lithium-sulfur (Li-S) batteries. However, it remains challenging to probe the sulfur redox reactions and mechanism at the electrocatalyst/LiPS interface after the active sites are covered by the solid discharge products LiS/LiS. Here, we demonstrate the intrinsic autocatalytic activity of the LiS (100) plane towards lithium polysulfides on single-atom nickel (SANi) electrocatalysts. Guided by theoretical models and experimental data, it is concluded that LiPS dissociates into LiS and short-chain LiPS on the LiS (100) plane. Subsequently, LiS undergoes further lithiation to LiS on the LiS (100) surface, generating a new LiS (100) layer, thus enabling the autocatalytic formation of a new LiS (100) surface. Benefiting from the autocatalytic growth of LiS, the concentration of LiPS in the electrolyte remains at a lower level, enabling Li-S batteries under high loading and low electrolyte conditions to exhibit superior electrochemical performance.

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Source
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC11535435PMC
http://dx.doi.org/10.1038/s41467-024-53797-yDOI Listing

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