{"title":"醚基功能化离子液体在锂硫电池中的相互作用：第一性原理研究。","authors":"Chengren Li, Nan Zhou, Jiaxin Tang, Chen Wang, Rongde Sun, Baifeng Yang, Zhigao Chen, Xiaohan Lu, Zhen Chang, Shaoze Zhang, Changjun Peng, Honglai Liu","doi":"10.1002/cphc.202400848","DOIUrl":null,"url":null,"abstract":"<p><p>Ionic liquids (ILs) as electrolytes in lithium-sulfur (Li-S) batteries effectively mitigate the shuttle effect. Solvated cationic ether-based ILs, comprising [Li(G1)<sub>2</sub>]<sup>+</sup>, [Li(G2)<sub>2</sub>]<sup>+</sup>, [LiG3]<sup>+</sup>, [LiG4]<sup>+</sup>, or [LiG6]<sup>+</sup> paired with bis(trifluoromethyllsulfonyl)imide ([TFSA]<sup>-</sup>) anions, are evaluated for their ability to suppress short-chain lithium polysulfide (LiPS: Li<sub>2</sub>S<sub>1</sub>, Li<sub>2</sub>S<sub>2</sub>, Li<sub>2</sub>S<sub>4</sub>) adsorption on lithium metal. The chelating capacity of solvated cations governs interactions with LiPSs and anions. Solvation via Li<sup>+</sup> chelation prevents free Li<sup>+</sup> fusion with LiPSs, reducing shuttle effects. Remarkably, the cyclic [LiG6]<sup>+</sup> cation exhibits superior Li<sup>+</sup> chelation, stability, and minimized LiPS adsorption compared to linear cations. Ab initio molecular dynamics simulations confirm ether-based ILs stabilize anions and lower LiPS-lithium surface reactivity. These findings highlight solvated cation ILs as tailored electrolytes to control interfacial LiPS behavior, advancing high-performance LiS battery design.</p>","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":" ","pages":"e2400848"},"PeriodicalIF":2.3000,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"The Interaction of Ether-Based Functionalized Ionic Liquids in Lithium-Sulfur Batteries: A First-Principles Study.\",\"authors\":\"Chengren Li, Nan Zhou, Jiaxin Tang, Chen Wang, Rongde Sun, Baifeng Yang, Zhigao Chen, Xiaohan Lu, Zhen Chang, Shaoze Zhang, Changjun Peng, Honglai Liu\",\"doi\":\"10.1002/cphc.202400848\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Ionic liquids (ILs) as electrolytes in lithium-sulfur (Li-S) batteries effectively mitigate the shuttle effect. Solvated cationic ether-based ILs, comprising [Li(G1)<sub>2</sub>]<sup>+</sup>, [Li(G2)<sub>2</sub>]<sup>+</sup>, [LiG3]<sup>+</sup>, [LiG4]<sup>+</sup>, or [LiG6]<sup>+</sup> paired with bis(trifluoromethyllsulfonyl)imide ([TFSA]<sup>-</sup>) anions, are evaluated for their ability to suppress short-chain lithium polysulfide (LiPS: Li<sub>2</sub>S<sub>1</sub>, Li<sub>2</sub>S<sub>2</sub>, Li<sub>2</sub>S<sub>4</sub>) adsorption on lithium metal. The chelating capacity of solvated cations governs interactions with LiPSs and anions. Solvation via Li<sup>+</sup> chelation prevents free Li<sup>+</sup> fusion with LiPSs, reducing shuttle effects. Remarkably, the cyclic [LiG6]<sup>+</sup> cation exhibits superior Li<sup>+</sup> chelation, stability, and minimized LiPS adsorption compared to linear cations. Ab initio molecular dynamics simulations confirm ether-based ILs stabilize anions and lower LiPS-lithium surface reactivity. These findings highlight solvated cation ILs as tailored electrolytes to control interfacial LiPS behavior, advancing high-performance LiS battery design.</p>\",\"PeriodicalId\":9819,\"journal\":{\"name\":\"Chemphyschem\",\"volume\":\" \",\"pages\":\"e2400848\"},\"PeriodicalIF\":2.3000,\"publicationDate\":\"2025-03-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemphyschem\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1002/cphc.202400848\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemphyschem","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1002/cphc.202400848","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
The Interaction of Ether-Based Functionalized Ionic Liquids in Lithium-Sulfur Batteries: A First-Principles Study.
Ionic liquids (ILs) as electrolytes in lithium-sulfur (Li-S) batteries effectively mitigate the shuttle effect. Solvated cationic ether-based ILs, comprising [Li(G1)2]+, [Li(G2)2]+, [LiG3]+, [LiG4]+, or [LiG6]+ paired with bis(trifluoromethyllsulfonyl)imide ([TFSA]-) anions, are evaluated for their ability to suppress short-chain lithium polysulfide (LiPS: Li2S1, Li2S2, Li2S4) adsorption on lithium metal. The chelating capacity of solvated cations governs interactions with LiPSs and anions. Solvation via Li+ chelation prevents free Li+ fusion with LiPSs, reducing shuttle effects. Remarkably, the cyclic [LiG6]+ cation exhibits superior Li+ chelation, stability, and minimized LiPS adsorption compared to linear cations. Ab initio molecular dynamics simulations confirm ether-based ILs stabilize anions and lower LiPS-lithium surface reactivity. These findings highlight solvated cation ILs as tailored electrolytes to control interfacial LiPS behavior, advancing high-performance LiS battery design.
期刊介绍：
ChemPhysChem is one of the leading chemistry/physics interdisciplinary journals (ISI Impact Factor 2018: 3.077) for physical chemistry and chemical physics. It is published on behalf of Chemistry Europe, an association of 16 European chemical societies.
ChemPhysChem is an international source for important primary and critical secondary information across the whole field of physical chemistry and chemical physics. It integrates this wide and flourishing field ranging from Solid State and Soft-Matter Research, Electro- and Photochemistry, Femtochemistry and Nanotechnology, Complex Systems, Single-Molecule Research, Clusters and Colloids, Catalysis and Surface Science, Biophysics and Physical Biochemistry, Atmospheric and Environmental Chemistry, and many more topics. ChemPhysChem is peer-reviewed.
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