Engineering d-p Orbital Hybridization with P, S Co-Coordination Asymmetric Configuration of Single Atoms Toward High-Rate and Long-Cycling Lithium-Sulfur Battery
© 2024 Wiley‐VCH GmbH.
Publié dans: | Advanced materials (Deerfield Beach, Fla.). - 1998. - 36(2024), 38 vom: 01. Sept., Seite e2407070 |
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Auteur principal: | |
Autres auteurs: | , , , , , , , , , , , |
Format: | Article en ligne |
Langue: | English |
Publié: |
2024
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Accès à la collection: | Advanced materials (Deerfield Beach, Fla.) |
Sujets: | Journal Article coordination regulation electrocatalysis lithium–sulfur batteries single atom catalyst |
Résumé: | © 2024 Wiley‐VCH GmbH. Single-atom catalysts (SACs) have been increasingly explored in lithium-sulfur (Li-S) batteries to address the issues of severe polysulfide shuttle effects and sluggish redox kinetics. However, the structure-activity relationship between single-atom coordination structures and the performance of Li-S batteries remain unclear. In this study, a P, S co-coordination asymmetric configuration of single atoms is designed to enhance the catalytic activity of Co central atoms and promote d-p orbital hybridization between Co and S atoms, thereby limiting polysulfides and accelerating the bidirectional redox process of sulfur. The well-designed SACs enable Li-S batteries to demonstrate an ultralow capacity fading rate of 0.027% per cycle after 2000 cycles at a high rate of 5 C. Furthermore, they display excellent rate performance with a capacity of 619 mAh g-1 at an ultrahigh rate of 10 C due to the efficient catalysis of CoSA-N3PS. Importantly, the assembled pouch cell still retains a high discharge capacity of 660 mAh g-1 after 100 cycles at 0.2 C and provides a high areal capacity of 4.4 mAh cm-2 even with a high sulfur loading of 6 mg cm-2. This work demonstrates that regulating the coordination environment of SACs is of great significance for achieving state-of-the-art Li-S batteries |
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Description: | Date Revised 03.10.2024 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
ISSN: | 1521-4095 |
DOI: | 10.1002/adma.202407070 |