A Click Chemistry Strategy Toward Spin-Polarized Transition-Metal Single Site Catalysts for Dynamic Probing of Sulfur Redox Electrocatalysis
© 2024 Wiley‐VCH GmbH.
| Veröffentlicht in: | Advanced materials (Deerfield Beach, Fla.). - 1998. - (2024) vom: 17. Sept., Seite e2409369 |
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| 1. Verfasser: | |
| Weitere Verfasser: | , , , , , , , |
| Format: | Online-Aufsatz |
| Sprache: | English |
| Veröffentlicht: |
2024
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| Zugriff auf das übergeordnete Werk: | Advanced materials (Deerfield Beach, Fla.) |
| Schlagworte: | Journal Article Li–S batteries metallophthalocyanines single site catalysts spin state sulfur redox reactions |
| Zusammenfassung: | © 2024 Wiley‐VCH GmbH. Catalytic conversion of lithium polysulfides (LiPSs) is a crucial approach to enhance the redox kinetics and suppress the shuttle effect in lithium-sulfur (Li-S) batteries. However, the roles of a typical heterogenous catalyst cannot be easily identified due to its structural complexity. Compared with the distinct sites of single atom catalysts (SACs), each active site of single site catalysts (SSCs) is identical and uniform in their spatial energy, binding mode, and coordination sphere, etc. Benefiting from the well-defined structure, iron phthalocyanine (FePc) is covalently clicked onto CuO nanosheet to prepare low spin-state Fe SSCs as the model catalyst for Li-S electrochemistry. The periodic polarizability evolution of Fe-N bonding is probed during sulfur redox reaction by in situ Raman spectra. Theoretical analysis shows the decreased d-band center gap of Fe (Δd) and delocalization of dxz/dyz after the axial click confinement. Consequently, Li-S batteries with Fe SSCs exhibit a capacity decay rate of 0.029% per cycle at 2 C. The universality of this methodological approach is demonstrated by a series of M SSCs (M = Mn, Co, and Ni) with similar variation of electronic configuration. This work provides guidance for the design of efficient electrocatalysis in Li-S batteries |
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| Beschreibung: | Date Revised 17.09.2024 published: Print-Electronic Citation Status Publisher |
| ISSN: | 1521-4095 |
| DOI: | 10.1002/adma.202409369 |