4.8 Review

Electrocatalyst Modulation toward Bidirectional Sulfur Redox in Li-S Batteries: From Strategic Probing to Mechanistic Understanding

Journal

ADVANCED ENERGY MATERIALS
Volume 12, Issue 29, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.202201056

Keywords

bidirectional redox kinetics; electrocatalyst modulation; Li; S-2 nucleation; Li-S batteries; polysulfide conversion

Funding

  1. National Natural Science Foundation of China [22179089]
  2. Science Fund for Distinguished Young Scholars of Jiangsu Province [BK20211503]
  3. Suzhou Science and Technology Project-Prospective Application Research Program [SYG202038]
  4. Suzhou Key Laboratory for Advanced Carbon Materials and Wearable Energy Technologies, Suzhou, China

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This article summarizes emerging strategies in the modulation of heterogeneous and homogeneous electrocatalysts, emphasizes the importance of deciphering bidirectional sulfur electrochemistry, and proposes a 3s electrocatalysis model to deepen understanding of the sulfur electrocatalytic mechanism.
Electrocatalyst design has stimulated considerable attention and strenuous effort to tackle a multitude of detrimental issues in lithium-sulfur (Li-S) systems, mainly pertaining to the severe polysulfide shuttle effect and sluggish sulfur redox kinetics. In this context related advances in expediting bidirectional sulfur reactions have lately surged. Nonetheless, the structure-activity correlation and electrocatalytic mechanism remain rather elusive, as a result of elusory active sites, complicated aprotic environments, and multistep conversion pathways. This review summarizes burgeoning strategies in the modulation of heterogeneous and homogeneous electrocatalysts, wherein the advanced electrokinetic measurements, operando instrumental probing, and theoretical simulations are elucidated with an emphasis on deciphering bidirectional sulfur electrochemistry. Notably, a 3s electrocatalysis model is proposed to deepen the mechanistic understanding in this realm. Finally, a development roadmap is sketched and future research layouts are discussed, aiming in essence, to realize favorable bidirectional redox kinetics and ultimately bridge the gap between reality and ideal systems in working Li-S batteries.

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