Zhihua Wang, Junru Ke, He Zhu, Fan Xue, Jun Jiang, Wen Huang, Min Dong, Xindong Zhu, Jianrong Zeng, Ruoyu Song, Rafal Sliz, Qingmin Ji, Qi Liu, Yongsheng Fu, Si Lan
{"title":"位阻诱导的非晶硫化锂沉积加速了锂硫电池中硫的氧化还原动力学","authors":"Zhihua Wang, Junru Ke, He Zhu, Fan Xue, Jun Jiang, Wen Huang, Min Dong, Xindong Zhu, Jianrong Zeng, Ruoyu Song, Rafal Sliz, Qingmin Ji, Qi Liu, Yongsheng Fu, Si Lan","doi":"10.1002/adma.202504715","DOIUrl":null,"url":null,"abstract":"Lithium–sulfur (Li─S) batteries are promising candidates for next-generation energy storage due to their ultrahigh theoretical energy density. However, their practical application is severely hindered by the sluggish conversion kinetics, particularly during the crystalline lithium sulfide (Li<sub>2</sub>S) formation stage. Herein, a steric hindrance-mediated engineering strategy is proposed that induces an amorphous Li<sub>2</sub>S deposition process, effectively boosting the sulfur redox kinetics in Li─S batteries. By introducing benzo-15-crown-5 (B15C5) as an electrolyte additive, a strong coordination between B15C5 and lithium ion (Li<sup>+</sup>) is established, which creates spatial confinement around Li<sub>2</sub>S and disrupts the crystallinity of Li<sub>2</sub>S during its deposition. Synchrotron pair distribution function analysis combined with in situ X-ray diffraction reveals that the deposited Li<sub>2</sub>S with B15C5 exhibits significant local disorder with irregular Li─S bond oscillations, confirming the generation of an amorphous phase. This strategy not only ensures a uniform Li<sub>2</sub>S layer at the cathode/electrolyte interface but also lowers the energy barrier of sulfur species at the molecular scale, enabling the Li─S batteries with excellent cycling stability and overall enhanced sulfur reaction kinetics. This work provides a novel pathway for overcoming the intrinsic limitations of sluggish cathode conversion kinetics of Li─S batteries, paving the way for their practical deployment in high-performance energy storage applications.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"27 1","pages":""},"PeriodicalIF":27.4000,"publicationDate":"2025-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Steric Hindrance-Induced Amorphous Lithium Sulfide Deposition Accelerates Sulfur Redox Kinetics in Lithium–Sulfur Batteries\",\"authors\":\"Zhihua Wang, Junru Ke, He Zhu, Fan Xue, Jun Jiang, Wen Huang, Min Dong, Xindong Zhu, Jianrong Zeng, Ruoyu Song, Rafal Sliz, Qingmin Ji, Qi Liu, Yongsheng Fu, Si Lan\",\"doi\":\"10.1002/adma.202504715\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Lithium–sulfur (Li─S) batteries are promising candidates for next-generation energy storage due to their ultrahigh theoretical energy density. However, their practical application is severely hindered by the sluggish conversion kinetics, particularly during the crystalline lithium sulfide (Li<sub>2</sub>S) formation stage. Herein, a steric hindrance-mediated engineering strategy is proposed that induces an amorphous Li<sub>2</sub>S deposition process, effectively boosting the sulfur redox kinetics in Li─S batteries. By introducing benzo-15-crown-5 (B15C5) as an electrolyte additive, a strong coordination between B15C5 and lithium ion (Li<sup>+</sup>) is established, which creates spatial confinement around Li<sub>2</sub>S and disrupts the crystallinity of Li<sub>2</sub>S during its deposition. Synchrotron pair distribution function analysis combined with in situ X-ray diffraction reveals that the deposited Li<sub>2</sub>S with B15C5 exhibits significant local disorder with irregular Li─S bond oscillations, confirming the generation of an amorphous phase. This strategy not only ensures a uniform Li<sub>2</sub>S layer at the cathode/electrolyte interface but also lowers the energy barrier of sulfur species at the molecular scale, enabling the Li─S batteries with excellent cycling stability and overall enhanced sulfur reaction kinetics. This work provides a novel pathway for overcoming the intrinsic limitations of sluggish cathode conversion kinetics of Li─S batteries, paving the way for their practical deployment in high-performance energy storage applications.\",\"PeriodicalId\":114,\"journal\":{\"name\":\"Advanced Materials\",\"volume\":\"27 1\",\"pages\":\"\"},\"PeriodicalIF\":27.4000,\"publicationDate\":\"2025-05-13\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Advanced Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1002/adma.202504715\",\"RegionNum\":1,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1002/adma.202504715","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Lithium–sulfur (Li─S) batteries are promising candidates for next-generation energy storage due to their ultrahigh theoretical energy density. However, their practical application is severely hindered by the sluggish conversion kinetics, particularly during the crystalline lithium sulfide (Li2S) formation stage. Herein, a steric hindrance-mediated engineering strategy is proposed that induces an amorphous Li2S deposition process, effectively boosting the sulfur redox kinetics in Li─S batteries. By introducing benzo-15-crown-5 (B15C5) as an electrolyte additive, a strong coordination between B15C5 and lithium ion (Li+) is established, which creates spatial confinement around Li2S and disrupts the crystallinity of Li2S during its deposition. Synchrotron pair distribution function analysis combined with in situ X-ray diffraction reveals that the deposited Li2S with B15C5 exhibits significant local disorder with irregular Li─S bond oscillations, confirming the generation of an amorphous phase. This strategy not only ensures a uniform Li2S layer at the cathode/electrolyte interface but also lowers the energy barrier of sulfur species at the molecular scale, enabling the Li─S batteries with excellent cycling stability and overall enhanced sulfur reaction kinetics. This work provides a novel pathway for overcoming the intrinsic limitations of sluggish cathode conversion kinetics of Li─S batteries, paving the way for their practical deployment in high-performance energy storage applications.
期刊介绍:
Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.