Axial ligand induces the charge localization of Ca single-atom sites for efficient Na-S batteries.

IF 14.7 1区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES

Nature Communications Pub Date : 2025-05-12 DOI:10.1038/s41467-025-59437-3

Fangcai Zheng,Yuhang Zhang,Zhiqiang Li,Ge Yao,Lingzhi Wei,Changlai Wang,Qianwang Chen,Hui Wang

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Abstract

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-O4N-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 (Na2Sn) and simultaneously promotes the conversion kinetics. The Ca-O4N-C@S exhibits superior sulfur conversion activity of 1211 mAh g-1 based on the mass of sulfur at 335 mA g-1 after 100 cycles under a sulfur loading of 1.0 mg cm-2 with an electrolyte of 2M sodium bis(trifluoromethylsulfonyl)imide in propylene carbonate/fluoroethylene carbonate and an electrolyte-to-sulfur ratio of 70 μL mg-1, 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.

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轴向配体诱导高效钠硫电池中Ca单原子位的电荷定位。

主基团s-嵌段金属单原子催化剂（SACs）通常被认为对钠硫电池中的硫转化反应不具有催化活性。在此，我们设计了一个轴向N原子和四个平面O原子（Ca- o4n - c）配位的高效钙（Ca） SACs用于钠硫电池。轴向N配体诱导Ca位点的电荷定位，加强了Ca中心与硫种之间的p-p轨道杂化，增强了对多硫化钠（Na2Sn）的亲和力，同时促进了转化动力学。当含硫量为1.0 mg cm-2，电解液为2M的二（三氟甲基磺酰基）亚胺钠/氟乙烯碳酸酯，电解液硫比为70 μL mg-1时，Ca-O4N-C@S在循环100次后的硫质量为335 mA g-1，其硫转化活性为1211 mAh g-1，是钠硫电池的d块SACs的理想选择。本研究调节了高效钠硫电池中Ca sac的p轨道电荷分布。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Nature Communications Biological Science Disciplines-

CiteScore

24.90

自引率

2.40%

发文量

6928

审稿时长

3.7 months

期刊介绍： Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.