Junan Feng, Chaoyue Zhang, Wendong Liu, Shunxian Yu, Lei Wang, Tianyi Wang, Chuan Shi, Xiaoxian Zhao, Shuangqiang Chen, Shulei Chou, Jianjun Song
{"title":"通过制造抑制穿梭效应的双层功能化分离器,实现高效的锚定-转换界面。","authors":"Junan Feng, Chaoyue Zhang, Wendong Liu, Shunxian Yu, Lei Wang, Tianyi Wang, Chuan Shi, Xiaoxian Zhao, Shuangqiang Chen, Shulei Chou, Jianjun Song","doi":"10.1002/anie.202407042","DOIUrl":null,"url":null,"abstract":"<p><p>Lithium-sulfur batteries (LiSBs) with high energy density still face challenges on sluggish conversion kinetics, severe shuttle effects of lithium polysulfides (LiPSs), and low blocking feature of ordinary separators to LiPSs. To tackle these, a novel double-layer strategy to functionalize separators is proposed, which consists of Co with atomically dispersed CoN<sub>4</sub> decorated on Ketjen black (Co/CoN<sub>4</sub>@KB) layer and an ultrathin 2D Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> MXene layer. The theoretical calculations and experimental results jointly demonstrate metallic Co sites provide efficient adsorption and catalytic capability for long-chain LiPSs, while CoN<sub>4</sub> active sites facilitate the absorption of short-chain LiPSs and promote the conversion to Li<sub>2</sub>S. The stacking MXene layer serves as a microscopic barrier to further physically block and chemically anchor the leaked LiPSs from the pores and gaps of the Co/CoN<sub>4</sub>@KB layer, thus preserving LiPSs within efficient anchoring-conversion reaction interfaces to balance the accumulation of \"dead S\" and Li<sub>2</sub>S. Consequently, with an ultralight loading of Co/CoN<sub>4</sub>@KB-MXene, the LiSBs exhibit amazing electrochemical performance even under high sulfur loading and lean electrolyte, and the outperforming performance for lithium-selenium batteries (LiSeBs) can also be achieved. This work exploits a universal and effective strategy of a double-layer functionalized separator to regulate the equilibrium adsorption-catalytic interface, enabling high-energy and long-cycle LiSBs/LiSeBs.</p>","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":null,"pages":null},"PeriodicalIF":16.1000,"publicationDate":"2024-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Enabling Efficient Anchoring-Conversion Interface by Fabricating Double-Layer Functionalized Separator for Suppressing Shuttle Effect.\",\"authors\":\"Junan Feng, Chaoyue Zhang, Wendong Liu, Shunxian Yu, Lei Wang, Tianyi Wang, Chuan Shi, Xiaoxian Zhao, Shuangqiang Chen, Shulei Chou, Jianjun Song\",\"doi\":\"10.1002/anie.202407042\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Lithium-sulfur batteries (LiSBs) with high energy density still face challenges on sluggish conversion kinetics, severe shuttle effects of lithium polysulfides (LiPSs), and low blocking feature of ordinary separators to LiPSs. To tackle these, a novel double-layer strategy to functionalize separators is proposed, which consists of Co with atomically dispersed CoN<sub>4</sub> decorated on Ketjen black (Co/CoN<sub>4</sub>@KB) layer and an ultrathin 2D Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> MXene layer. The theoretical calculations and experimental results jointly demonstrate metallic Co sites provide efficient adsorption and catalytic capability for long-chain LiPSs, while CoN<sub>4</sub> active sites facilitate the absorption of short-chain LiPSs and promote the conversion to Li<sub>2</sub>S. The stacking MXene layer serves as a microscopic barrier to further physically block and chemically anchor the leaked LiPSs from the pores and gaps of the Co/CoN<sub>4</sub>@KB layer, thus preserving LiPSs within efficient anchoring-conversion reaction interfaces to balance the accumulation of \\\"dead S\\\" and Li<sub>2</sub>S. Consequently, with an ultralight loading of Co/CoN<sub>4</sub>@KB-MXene, the LiSBs exhibit amazing electrochemical performance even under high sulfur loading and lean electrolyte, and the outperforming performance for lithium-selenium batteries (LiSeBs) can also be achieved. This work exploits a universal and effective strategy of a double-layer functionalized separator to regulate the equilibrium adsorption-catalytic interface, enabling high-energy and long-cycle LiSBs/LiSeBs.</p>\",\"PeriodicalId\":125,\"journal\":{\"name\":\"Angewandte Chemie International Edition\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":16.1000,\"publicationDate\":\"2024-10-07\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Angewandte Chemie International Edition\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1002/anie.202407042\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2024/9/6 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Angewandte Chemie International Edition","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1002/anie.202407042","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2024/9/6 0:00:00","PubModel":"Epub","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Enabling Efficient Anchoring-Conversion Interface by Fabricating Double-Layer Functionalized Separator for Suppressing Shuttle Effect.
Lithium-sulfur batteries (LiSBs) with high energy density still face challenges on sluggish conversion kinetics, severe shuttle effects of lithium polysulfides (LiPSs), and low blocking feature of ordinary separators to LiPSs. To tackle these, a novel double-layer strategy to functionalize separators is proposed, which consists of Co with atomically dispersed CoN4 decorated on Ketjen black (Co/CoN4@KB) layer and an ultrathin 2D Ti3C2Tx MXene layer. The theoretical calculations and experimental results jointly demonstrate metallic Co sites provide efficient adsorption and catalytic capability for long-chain LiPSs, while CoN4 active sites facilitate the absorption of short-chain LiPSs and promote the conversion to Li2S. The stacking MXene layer serves as a microscopic barrier to further physically block and chemically anchor the leaked LiPSs from the pores and gaps of the Co/CoN4@KB layer, thus preserving LiPSs within efficient anchoring-conversion reaction interfaces to balance the accumulation of "dead S" and Li2S. Consequently, with an ultralight loading of Co/CoN4@KB-MXene, the LiSBs exhibit amazing electrochemical performance even under high sulfur loading and lean electrolyte, and the outperforming performance for lithium-selenium batteries (LiSeBs) can also be achieved. This work exploits a universal and effective strategy of a double-layer functionalized separator to regulate the equilibrium adsorption-catalytic interface, enabling high-energy and long-cycle LiSBs/LiSeBs.
期刊介绍:
Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.