Self-Assembled Macrocyclic Copper Complex Enables Homogeneous Catalysis for High-Loading Lithium-Sulfur Batteries
© 2023 Wiley-VCH GmbH.
| Publié dans: | Advanced materials (Deerfield Beach, Fla.). - 1998. - 35(2023), 26 vom: 15. Juni, Seite e2300861 |
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| Auteur principal: | |
| Autres auteurs: | , , , , |
| Format: | Article en ligne |
| Langue: | English |
| Publié: |
2023
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| Accès à la collection: | Advanced materials (Deerfield Beach, Fla.) |
| Sujets: | Journal Article Li-S batteries high-loading cathodes homogeneous catalysis macrocyclic cooper complexes self-assembly |
| Résumé: | © 2023 Wiley-VCH GmbH. The practical viability of high-energy-density lithium-sulfur (Li-S) batteries stipulates the use of a high-loading cathode and lean electrolyte. However, under such harsh conditions, the liquid-solid sulfur redox reaction is much retarded due to the poor sulfur and polysulfides utilization, leading to low capacity and fast fading. Herein, a self-assembled macrocyclic Cu(II) complex (CuL) is designed as an effective catalyst to homogenize and maximize the liquid-involving reaction. The Cu(II) ion coordinated with four N atoms features a planar d sp 2 ${\mathrm{d}}_{{\mathrm{sp}}^{2}}$ hybridization, showing a strong bonding affinity toward lithium polysulfides (LiPSs) along the d z 2 ${\mathrm{d}}_{{z}^{2}}$ orbital via steric effects. Such a structure not only lowers the energy barrier of the liquid-solid conversion (Li2 S4 to Li2 S2 ) but also guides a 3D deposition of Li2 S2 /Li2 S. As such, with a 1 wt% electrolyte additive of CuL, a high initial capacity of 925 mAh g-1 and areal capacity of 9.62 mAh cm-2 with a low decay of 0.3%/cycle can be achieved under a high sulfur loading of 10.4 mg cm-2 and low electrolyte/sulfur ratio of 6 µL mgs -1 . This work is expected to inspire the design of homogenous catalysts and accelerate the uptake of high-energy-density Li-S batteries |
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| Description: | Date Completed 28.06.2023 Date Revised 28.06.2023 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
| ISSN: | 1521-4095 |
| DOI: | 10.1002/adma.202300861 |