Accelerating sulfur redox kinetics by rare earth single-atom electrocatalysts toward efficient lithium–sulfur batteries

Toward practical lithium−sulfur (Li−S) batteries, there is a pressing need to improve the rate performance and longevity of cells. Herein, we report developing a cathode electrocatalyst Lu SA/NC, capable of accelerating sulfur redox kinetics with a high specific capacity of 1391.8 mAh g−1 at 0.1 C, and a low-capacity fading rate of 0.049 % per cycle over 1000 cycles even with a high sulfur loading (5.96 mg cm−2). The unparalleled cathodes are built upon the unique structure in which single-atoms of rare earth metals are doped in nitrogen-doped porous carbon (RM SAs/NC). The theoretical and experimental studies reveal that the rare earth Lu atom has an unrivaled adsorption capacity for polysulfides and can promote facile deposition and dissolution reactions in charge-discharge processes. The in-situ Raman experiments provide direct evidence for its promotion of polysulfide transformation to eliminate the shuttle effect. The theoretical calculations suggest that the presence of f-d-p hybridization enables accelerating sulfur reduction kinetics and enhancing lithium−sulfur battery performance. The strategic paradigm introduced in this study underscores significant practical potential in the exploration of rare earth single-atom catalysts for high performance Li−S batteries. © 2024 Elsevier B.V.