Energizing Robust Sulfur/Lithium Electrochemistry via Nanoscale-Asymmetric-Size Synergism

作者：Youzhang Huang, Jiantao Li, Yinggan Zhang, Liang Lin, Zhefei Sun, Guiyang Gao, Baisheng Sa, Laisen Wang, Lu Ma, Sungsik Lee, Ming‐Sheng Wang, Dong‐Liang Peng, Khalil Amine, Qingshui Xie · 发表于：Journal of the American Chemical Society · 年份：2025 · DOI：10.1021/jacs.4c10238 · 被引用次数：41 · 研究领域：Advanced Battery Materials and Technologies、Advancements in Battery Materials、Thermal Expansion and Ionic Conductivity

Sluggish redox kinetics and dendrite growth perplex the fulfillment of efficient electrochemistry in lithium–sulfur (Li–S) batteries. The complicated sulfur phase transformation and sulfur/lithium diversity kinetics necessitate an all-inclusive approach in catalyst design. Herein, a compatible mediator with nanoscale-asymmetric-size configuration by integrating Co single atoms and defective CoTe 2– x (Co SA -CoTe 2– x @NHCF) is elaborately developed for regulating sulfur/lithium electrochemistry synchronously. Substantial electrochemistry and theoretical analyses reveal that CoTe 2– x exhibits higher catalytic activity in long-chain polysulfide transformation and Li 2 S decomposition, while monodispersed Co sites are more effective in boosting sulfur reduction kinetics to regulate Li 2 S deposition. Such cascade catalysis endows Co SA -CoTe 2– x @NHCF with the all-around service of “trapping-conversion-recuperation” for sulfur species during the whole redox reaction. Furthermore, it is demonstrated by in situ transmission electron microscopy that initially formed electronic-conductive Co and ionic-conductive Li 2 Te provide sufficient lithiophilic sites to regulate homogeneous Li plating and stripping with markedly suppressed dendrite growth. Consequently, by coupling the Co SA -CoTe 2– x @NHCF interlayer and Li@Co SA -CoTe 2– x @NHCF anode, the constructed Li–S full batteries deliver superior cycling stability and rate performance, and the flexible pouch cell exhibits stable...