Interfacial "Double-Terminal Binding Sites" Catalysts Synergistically Boosting the Electrocatalytic Li2S Redox for Durable Lithium-Sulfur Batteries
Catalytic conversion of polysulfides emerges as a promising approach to improve the kinetics and mitigate polysulfide shuttling in lithium-sulfur (Li-S) batteries, especially under conditions of high sulfur loading and lean electrolyte. Herein, we present a separator architecture that incorporates double-terminal binding (DTB) sites within a nitrogen-doped carbon framework, consisting of polar Co0.85Se and Co clusters (Co/Co0.85SeNC), to enhance the durability of Li-S batteries. The uniformly dispersed clusters of polar Co0.85Se and Co offer abundant active sites for lithium polysulfides (LiPSs), enabling efficient LiPS conversion while also serving as anchors through a combination of chemical interactions. Density functional theory calculations, along with in situ Raman and X-ray diffraction characterizations, reveal that the DTB effect strengthens the binding energy to polysulfides and lowers the energy barriers of polysulfide redox reactions. Li-S batteries utilizing the Co/Co0.85Se@NC-modified separator demonstrate exceptional cycling stability (0.042% per cycle over 1000 cycles at 2 C) and rate capability (849 mAh g-1 at 3 C), as well as deliver an impressive areal capacity of 10.0 mAh cm-2 even in challenging conditions with a high sulfur loading (10.7 mg cm-2) and lean electrolyte environments (5.8 μL mg-1). The DTB site strategy offers valuable insights into the development of high-performance Li-S batteries.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2024 |
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| Erschienen: |
2024 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:18 |
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| Enthalten in: |
ACS nano - 18(2024), 12 vom: 26. März, Seite 8839-8852 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Xu, Huifang [VerfasserIn] |
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| Links: |
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| Themen: |
Binding energy |
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| Anmerkungen: |
Date Revised 30.03.2024 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
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| doi: |
10.1021/acsnano.3c11903 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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| 520 | |a Catalytic conversion of polysulfides emerges as a promising approach to improve the kinetics and mitigate polysulfide shuttling in lithium-sulfur (Li-S) batteries, especially under conditions of high sulfur loading and lean electrolyte. Herein, we present a separator architecture that incorporates double-terminal binding (DTB) sites within a nitrogen-doped carbon framework, consisting of polar Co0.85Se and Co clusters (Co/Co0.85SeNC), to enhance the durability of Li-S batteries. The uniformly dispersed clusters of polar Co0.85Se and Co offer abundant active sites for lithium polysulfides (LiPSs), enabling efficient LiPS conversion while also serving as anchors through a combination of chemical interactions. Density functional theory calculations, along with in situ Raman and X-ray diffraction characterizations, reveal that the DTB effect strengthens the binding energy to polysulfides and lowers the energy barriers of polysulfide redox reactions. Li-S batteries utilizing the Co/Co0.85Se@NC-modified separator demonstrate exceptional cycling stability (0.042% per cycle over 1000 cycles at 2 C) and rate capability (849 mAh g-1 at 3 C), as well as deliver an impressive areal capacity of 10.0 mAh cm-2 even in challenging conditions with a high sulfur loading (10.7 mg cm-2) and lean electrolyte environments (5.8 μL mg-1). The DTB site strategy offers valuable insights into the development of high-performance Li-S batteries | ||
| 650 | 4 | |a Journal Article | |
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| 650 | 4 | |a double-terminal binding sites | |
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| 650 | 4 | |a superb electrocatalysis | |
| 700 | 1 | |a Jiang, Qingbin |e verfasserin |4 aut | |
| 700 | 1 | |a Hui, Kwan San |e verfasserin |4 aut | |
| 700 | 1 | |a Wang, Shuo |e verfasserin |4 aut | |
| 700 | 1 | |a Liu, Lingwen |e verfasserin |4 aut | |
| 700 | 1 | |a Chen, Tianyu |e verfasserin |4 aut | |
| 700 | 1 | |a Zheng, Yunshan |e verfasserin |4 aut | |
| 700 | 1 | |a Ip, Weng Fai |e verfasserin |4 aut | |
| 700 | 1 | |a Dinh, Duc Anh |e verfasserin |4 aut | |
| 700 | 1 | |a Zha, Chenyang |e verfasserin |4 aut | |
| 700 | 1 | |a Lin, Zhan |e verfasserin |4 aut | |
| 700 | 1 | |a Hui, Kwun Nam |e verfasserin |4 aut | |
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