Zheng Fangcai, Zhang Yuhang, Li Zhiqiang, Yao Ge, Wei Lingzhi, Wang Changlai, Chen Qianwang, Wang Hui
High Magnetic Field Laboratory, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Hefei, Anhui, 230031, P. R. China.
Institutes of Physical Science and Information Technology, Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education, Anhui University, Hefei, 230601, P. R. China.
Nat Commun. 2025 May 12;16(1):4372. doi: 10.1038/s41467-025-59437-3.
The main-group s-block metal single-atom catalysts (SACs) are typically regarded as catalytically inactive for sulfur conversion reactions in sodium-sulfur batteries. Herein, we design efficient calcium (Ca) SACs coordinated with one axial N atom and four planar O atoms (Ca-ON-C) for sodium-sulfur batteries. The axial N ligand induces the charge localization at Ca sites to strengthen p-p orbital-hybridization between Ca centers and sulfur species, which boosts the affinity toward sodium polysulfides (NaS) and simultaneously promotes the conversion kinetics. The Ca-ON-C@S exhibits superior sulfur conversion activity of 1211 mAh g based on the mass of sulfur at 335 mA g after 100 cycles under a sulfur loading of 1.0 mg cm with an electrolyte of 2M sodium bis(trifluoromethylsulfonyl)imide in propylene carbonate/fluoroethylene carbonate and an electrolyte-to-sulfur ratio of 70 μL mg, which is well-placed among d-block SACs for sodium-sulfur batteries. This work regulates the p orbital charge distribution of Ca SACs for efficient sodium-sulfur batteries.
主族s区金属单原子催化剂（SACs）通常被认为对钠硫电池中的硫转化反应没有催化活性。在此，我们设计了一种高效的钙（Ca）单原子催化剂，其与一个轴向N原子和四个平面O原子配位（Ca-ON-C）用于钠硫电池。轴向N配体诱导电荷定位于Ca位点，以加强Ca中心与硫物种之间的p-p轨道杂化，这增强了对多硫化钠（NaS）的亲和力，同时促进了转化动力学。在1.0 mg cm²的硫负载量、2M双（三氟甲基磺酰）亚胺钠在碳酸丙烯酯/氟代碳酸乙烯酯中的电解液以及70 μL mg的电解液与硫的比例条件下，Ca-ON-C@S在335 mA g的电流密度下循环100次后基于硫的质量表现出1211 mAh g的优异硫转化活性，在用于钠硫电池的d区单原子催化剂中处于良好水平。这项工作调节了Ca单原子催化剂的p轨道电荷分布以实现高效的钠硫电池。
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