Heteroatom‐Synergistic Effect on Anchoring Polysulfides In Chalcone‐Linked Nanographene Covalent Organic Frameworks for High‐Performance Li─S Batteries
Abstract Lithium‐sulfur (Li─S) batteries are an attractive option for future energy storage devices because they offer higher theoretical specific capacity, energy density, and cost‐effectiveness than commercial lithium‐ion batteries. However, the practical applications of Li─S batteries are signifi...
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Wiley
2025-04-01
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| Series: | Advanced Science |
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| Online Access: | https://doi.org/10.1002/advs.202415897 |
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| author | Kayaramkodath Chandran Ranjeesh Bharathkumar H. Javaregowda Safa Gaber Preeti Bhauriyal Sushil Kumar Tina Skorjanc Matjaž Finšgar Thomas Heine Kothandam Krishnamoorthy Dinesh Shetty |
| author_facet | Kayaramkodath Chandran Ranjeesh Bharathkumar H. Javaregowda Safa Gaber Preeti Bhauriyal Sushil Kumar Tina Skorjanc Matjaž Finšgar Thomas Heine Kothandam Krishnamoorthy Dinesh Shetty |
| author_sort | Kayaramkodath Chandran Ranjeesh |
| collection | DOAJ |
| description | Abstract Lithium‐sulfur (Li─S) batteries are an attractive option for future energy storage devices because they offer higher theoretical specific capacity, energy density, and cost‐effectiveness than commercial lithium‐ion batteries. However, the practical applications of Li─S batteries are significantly limited by the shuttle effect caused by intermediate lithium polysulfides (LiPSs) and slow redox kinetics. In this study, the molecular engineering of chalcone‐linked, sp2‐bonded nanographene‐type covalent organic frameworks (COFs) as sulfur hosts is reported to enhance interactions with LiPSs, thereby effectively suppressing the shuttle effect. The developed sulfur‐hosting cathode material demonstrated outstanding battery performance, surpassing most reported materials by achieving a specific capacity of 1228 mA h g−1 at 0.5C, with 80% retention after 500 cycles and an average Coulombic Efficiency (C.E.) of 99%. Additionally, the mechanisms of sulfur immobilization, the subsequent conversion into lithium polysulfides (LiPSs), and their binding energies with COFs are investigated using density functional theory (DFT) calculations. These findings offer valuable insights into the structure‐property relationships essential for developing more efficient sulfur‐hosting cathodes. |
| format | Article |
| id | doaj-art-bf2d4410488b4d139546aa30cea95131 |
| institution | OA Journals |
| issn | 2198-3844 |
| language | English |
| publishDate | 2025-04-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj-art-bf2d4410488b4d139546aa30cea951312025-08-20T02:24:50ZengWileyAdvanced Science2198-38442025-04-011216n/an/a10.1002/advs.202415897Heteroatom‐Synergistic Effect on Anchoring Polysulfides In Chalcone‐Linked Nanographene Covalent Organic Frameworks for High‐Performance Li─S BatteriesKayaramkodath Chandran Ranjeesh0Bharathkumar H. Javaregowda1Safa Gaber2Preeti Bhauriyal3Sushil Kumar4Tina Skorjanc5Matjaž Finšgar6Thomas Heine7Kothandam Krishnamoorthy8Dinesh Shetty9Department of Chemistry Khalifa University of Science & Technology Abu Dhabi P.O. Box 127788 UAEPolymer Science and Engineering Division, CSIR‐National Chemical Laboratory (CSIR‐NCL) Pune 411008 IndiaDepartment of Chemistry Khalifa University of Science & Technology Abu Dhabi P.O. Box 127788 UAEFaculty of Chemistry and Food Chemistry Technische Universität Dresden 01062 Dresden GermanyDepartment of Chemistry Khalifa University of Science & Technology Abu Dhabi P.O. Box 127788 UAEMaterials Research Laboratory University of Nova Gorica Vipavska cesta 11c Ajdovscina 5270 SloveniaFaculty of Chemistry and Chemical Engineering University of Maribor Smetanova ulica 17 Maribor 2000 SloveniaFaculty of Chemistry and Food Chemistry Technische Universität Dresden 01062 Dresden GermanyPolymer Science and Engineering Division, CSIR‐National Chemical Laboratory (CSIR‐NCL) Pune 411008 IndiaDepartment of Chemistry Khalifa University of Science & Technology Abu Dhabi P.O. Box 127788 UAEAbstract Lithium‐sulfur (Li─S) batteries are an attractive option for future energy storage devices because they offer higher theoretical specific capacity, energy density, and cost‐effectiveness than commercial lithium‐ion batteries. However, the practical applications of Li─S batteries are significantly limited by the shuttle effect caused by intermediate lithium polysulfides (LiPSs) and slow redox kinetics. In this study, the molecular engineering of chalcone‐linked, sp2‐bonded nanographene‐type covalent organic frameworks (COFs) as sulfur hosts is reported to enhance interactions with LiPSs, thereby effectively suppressing the shuttle effect. The developed sulfur‐hosting cathode material demonstrated outstanding battery performance, surpassing most reported materials by achieving a specific capacity of 1228 mA h g−1 at 0.5C, with 80% retention after 500 cycles and an average Coulombic Efficiency (C.E.) of 99%. Additionally, the mechanisms of sulfur immobilization, the subsequent conversion into lithium polysulfides (LiPSs), and their binding energies with COFs are investigated using density functional theory (DFT) calculations. These findings offer valuable insights into the structure‐property relationships essential for developing more efficient sulfur‐hosting cathodes.https://doi.org/10.1002/advs.202415897covalent organic frameworkslithium‐sulfur batterynanographeneanion‐pi interactionpolysulfide shuttle |
| spellingShingle | Kayaramkodath Chandran Ranjeesh Bharathkumar H. Javaregowda Safa Gaber Preeti Bhauriyal Sushil Kumar Tina Skorjanc Matjaž Finšgar Thomas Heine Kothandam Krishnamoorthy Dinesh Shetty Heteroatom‐Synergistic Effect on Anchoring Polysulfides In Chalcone‐Linked Nanographene Covalent Organic Frameworks for High‐Performance Li─S Batteries Advanced Science covalent organic frameworks lithium‐sulfur battery nanographene anion‐pi interaction polysulfide shuttle |
| title | Heteroatom‐Synergistic Effect on Anchoring Polysulfides In Chalcone‐Linked Nanographene Covalent Organic Frameworks for High‐Performance Li─S Batteries |
| title_full | Heteroatom‐Synergistic Effect on Anchoring Polysulfides In Chalcone‐Linked Nanographene Covalent Organic Frameworks for High‐Performance Li─S Batteries |
| title_fullStr | Heteroatom‐Synergistic Effect on Anchoring Polysulfides In Chalcone‐Linked Nanographene Covalent Organic Frameworks for High‐Performance Li─S Batteries |
| title_full_unstemmed | Heteroatom‐Synergistic Effect on Anchoring Polysulfides In Chalcone‐Linked Nanographene Covalent Organic Frameworks for High‐Performance Li─S Batteries |
| title_short | Heteroatom‐Synergistic Effect on Anchoring Polysulfides In Chalcone‐Linked Nanographene Covalent Organic Frameworks for High‐Performance Li─S Batteries |
| title_sort | heteroatom synergistic effect on anchoring polysulfides in chalcone linked nanographene covalent organic frameworks for high performance li─s batteries |
| topic | covalent organic frameworks lithium‐sulfur battery nanographene anion‐pi interaction polysulfide shuttle |
| url | https://doi.org/10.1002/advs.202415897 |
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