Electrocatalyst Modulation toward Bidirectional Sulfur Redox in Li–S Batteries: From Strategic Probing to Mechanistic Understanding. Issue 29 (7th June 2022)

• Record Type: Journal Article
• Authors: Shi, Zixiong; Ding, Yifan; Zhang, Qiang; Sun, Jingyu
• Is Part Of: Advanced energy materials. Volume 12:Issue 29(2022)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2022-06-07
• Subjects: bidirectional redox kinetics -- electrocatalyst modulation -- Li 2S nucleation -- Li–S batteries -- polysulfide conversion; Energy harvesting -- Materials -- Periodicals; Energy conversion -- Materials -- Periodicals; Energy storage -- Materials -- Periodicals; Photovoltaics -- Periodicals; Fuel cells -- Periodicals; Thermoelectric materials -- Periodicals; 621.31
• DOI: 10.1002/aenm.202201056
• Languages: English
• ISSNs: 1614-6832

Abstract

Abstract: 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. Abstract : Bidirectional electrocatalysts have stimulated a burgeoning interest in enhancing sulfur redox kinetics in lithium–sulfur (Li–S) batteries. In this review the many modulation strategies for heterogeneous and homogeneous electrocatalysts are comprehensively summarized. Furthermore, the underlying electrocatalytic mechanism for expediting bidirectional Li–S chemistry is discussed. Finally, promising research directions are presented.