{"title":"2,6-二羟基蒽醌与Co原子协同作用提高锂硫电池中多硫转化","authors":"Huijuan You, Fangfang Liu, Hanxiao Wang, Zining Wang, Xuyun Wang*, Boshen Zhang, Kuanshuo Tang, Jianwei Ren* and Rongfang Wang*, ","doi":"10.1021/acssuschemeng.4c0922810.1021/acssuschemeng.4c09228","DOIUrl":null,"url":null,"abstract":"<p >Currently, lithium–sulfur batteries for wider applications are challenged by both the shuttle effect in the cathodes as well as the slow kinetics of the sulfur redox reactions. Although metal compounds have been reported to suppress the shuttle effect of lithium polysulfides (LiPSs) by chemically adsorbing LiPSs and catalyzing their conversion, current methods for sulfur fixation on cathode materials remain insufficient. In this work, 2,6-dihydroxyanthraquinone (DHAQ) is tightly adsorbed on a Co-doped porous carbon (Co–C) substrate through π–π stacking. The abundant oxygen-containing functional groups in DHAQ form Li–O bonds with lithium in the LiPSs and enable in situ covalent fixation. Meanwhile, cobalt in Co–C forms Co–S bonds with sulfur in LiPSs, providing an efficient pathway for electron transfer and promoting LiPS conversion. Thus, the DHAQ/Co–C composite provides dual chemical adsorption capabilities that mitigate the “shuttle effect” of LiPSs. Additionally, the conductive merits of the DHAQ and Co–C networks accelerate electron transfer, enhance LiPS redox kinetics, and increase the battery’s specific capacity. In the end, the optimized S@DHAQ/Co–C composite demonstrates an initial discharge capacity (1385 mAh g<sup>–1</sup>) at 0.1C. After 600 cycles, the electrode displays a capacity decay rate of 0.062% at 1C. Compared with metal-based materials that rely solely on chemical sulfur fixation, the synergistic effect of organic oxygen atoms and metals in sulfur fixation offers significant improvements.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 5","pages":"2154–2163 2154–2163"},"PeriodicalIF":7.3000,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Enhancing Polysulfide Conversion in Lithium–Sulfur Batteries through the Synergistic Effect of 2,6-Dihydroxyanthraquinone and Co Atoms\",\"authors\":\"Huijuan You, Fangfang Liu, Hanxiao Wang, Zining Wang, Xuyun Wang*, Boshen Zhang, Kuanshuo Tang, Jianwei Ren* and Rongfang Wang*, \",\"doi\":\"10.1021/acssuschemeng.4c0922810.1021/acssuschemeng.4c09228\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Currently, lithium–sulfur batteries for wider applications are challenged by both the shuttle effect in the cathodes as well as the slow kinetics of the sulfur redox reactions. Although metal compounds have been reported to suppress the shuttle effect of lithium polysulfides (LiPSs) by chemically adsorbing LiPSs and catalyzing their conversion, current methods for sulfur fixation on cathode materials remain insufficient. In this work, 2,6-dihydroxyanthraquinone (DHAQ) is tightly adsorbed on a Co-doped porous carbon (Co–C) substrate through π–π stacking. The abundant oxygen-containing functional groups in DHAQ form Li–O bonds with lithium in the LiPSs and enable in situ covalent fixation. Meanwhile, cobalt in Co–C forms Co–S bonds with sulfur in LiPSs, providing an efficient pathway for electron transfer and promoting LiPS conversion. Thus, the DHAQ/Co–C composite provides dual chemical adsorption capabilities that mitigate the “shuttle effect” of LiPSs. Additionally, the conductive merits of the DHAQ and Co–C networks accelerate electron transfer, enhance LiPS redox kinetics, and increase the battery’s specific capacity. In the end, the optimized S@DHAQ/Co–C composite demonstrates an initial discharge capacity (1385 mAh g<sup>–1</sup>) at 0.1C. After 600 cycles, the electrode displays a capacity decay rate of 0.062% at 1C. Compared with metal-based materials that rely solely on chemical sulfur fixation, the synergistic effect of organic oxygen atoms and metals in sulfur fixation offers significant improvements.</p>\",\"PeriodicalId\":25,\"journal\":{\"name\":\"ACS Sustainable Chemistry & Engineering\",\"volume\":\"13 5\",\"pages\":\"2154–2163 2154–2163\"},\"PeriodicalIF\":7.3000,\"publicationDate\":\"2025-01-27\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Sustainable Chemistry & Engineering\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acssuschemeng.4c09228\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Sustainable Chemistry & Engineering","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acssuschemeng.4c09228","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
目前,锂硫电池的广泛应用受到阴极穿梭效应和硫氧化还原反应缓慢动力学的挑战。虽然有报道称金属化合物通过化学吸附多硫化物锂并催化其转化来抑制多硫化物锂的穿梭效应,但目前在正极材料上固硫的方法仍然不足。在这项工作中,2,6-二羟基蒽醌(DHAQ)通过π -π堆叠紧密吸附在共掺杂多孔碳(Co-C)衬底上。DHAQ中丰富的含氧官能团与LiPSs中的锂形成Li-O键,实现原位共价固定。同时,Co-C中的钴与LiPSs中的硫形成Co-S键,为电子转移提供了有效途径,促进了LiPS的转化。因此,DHAQ/ Co-C复合材料提供了双重化学吸附能力,减轻了LiPSs的“穿梭效应”。此外,DHAQ和Co-C网络的导电优点加速了电子转移,增强了LiPS氧化还原动力学,并增加了电池的比容量。最后,优化后的S@DHAQ/ Co-C复合材料在0.1C下的初始放电容量为1385 mAh g-1。经过600次循环,电极在1C下的容量衰减率为0.062%。与单纯依靠化学固硫的金属基材料相比,有机氧原子与金属在固硫中的协同作用有了显著的提高。
Enhancing Polysulfide Conversion in Lithium–Sulfur Batteries through the Synergistic Effect of 2,6-Dihydroxyanthraquinone and Co Atoms
Currently, lithium–sulfur batteries for wider applications are challenged by both the shuttle effect in the cathodes as well as the slow kinetics of the sulfur redox reactions. Although metal compounds have been reported to suppress the shuttle effect of lithium polysulfides (LiPSs) by chemically adsorbing LiPSs and catalyzing their conversion, current methods for sulfur fixation on cathode materials remain insufficient. In this work, 2,6-dihydroxyanthraquinone (DHAQ) is tightly adsorbed on a Co-doped porous carbon (Co–C) substrate through π–π stacking. The abundant oxygen-containing functional groups in DHAQ form Li–O bonds with lithium in the LiPSs and enable in situ covalent fixation. Meanwhile, cobalt in Co–C forms Co–S bonds with sulfur in LiPSs, providing an efficient pathway for electron transfer and promoting LiPS conversion. Thus, the DHAQ/Co–C composite provides dual chemical adsorption capabilities that mitigate the “shuttle effect” of LiPSs. Additionally, the conductive merits of the DHAQ and Co–C networks accelerate electron transfer, enhance LiPS redox kinetics, and increase the battery’s specific capacity. In the end, the optimized S@DHAQ/Co–C composite demonstrates an initial discharge capacity (1385 mAh g–1) at 0.1C. After 600 cycles, the electrode displays a capacity decay rate of 0.062% at 1C. Compared with metal-based materials that rely solely on chemical sulfur fixation, the synergistic effect of organic oxygen atoms and metals in sulfur fixation offers significant improvements.
期刊介绍:
ACS Sustainable Chemistry & Engineering is a prestigious weekly peer-reviewed scientific journal published by the American Chemical Society. Dedicated to advancing the principles of green chemistry and green engineering, it covers a wide array of research topics including green chemistry, green engineering, biomass, alternative energy, and life cycle assessment.
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