Rationally Reconstructed Metal-Organic Frameworks as Robust Oxygen Evolution Electrocatalysts
© 2022 Wiley-VCH GmbH.
| Veröffentlicht in: | Advanced materials (Deerfield Beach, Fla.). - 1998. - 35(2023), 8 vom: 20. Feb., Seite e2208904 |
|---|---|
| 1. Verfasser: | |
| Weitere Verfasser: | , , , , , , , |
| Format: | Online-Aufsatz |
| Sprache: | English |
| Veröffentlicht: |
2023
|
| Zugriff auf das übergeordnete Werk: | Advanced materials (Deerfield Beach, Fla.) |
| Schlagworte: | Journal Article electrocatalysis metal-organic frameworks oxygen evolution reaction real-time kinetic simulation reconstruction |
| Zusammenfassung: | © 2022 Wiley-VCH GmbH. Reconstructing metal-organic framework (MOFs) toward a designed framework structure provides breakthrough opportunities to achieve unprecedented oxygen evolution reaction (OER) electrocatalytic performance, but has rarely, if ever, been proposed and investigated yet. Here, the first successful fabrication of a robust OER electrocatalyst by precision reconstruction of an MOF structure is reported, viz., from MOF-74-Fe to MIL-53(Fe)-2OH with different coordination environments at the active sites. Due to the radically reduced eg -t2g crystal-field splitting in Fe-3d and the much suppressed electron-hopping barriers through the synergistic effects of the O species the efficient OER of in MIL-53(Fe)-2OH is guaranteed. Benefiting from this desired electronic structure, the designed MIL-53(Fe)-2OH catalyst exhibits high intrinsic OER activity, including a low overpotential of 215 mV at 10 mA cm-2 , low Tafel slope of 45.4 mV dec-1 and high turnover frequency (TOF) of 1.44 s-1 at 300 mV overpotential, over 80 times that of the commercial IrO2 catalyst (0.0177 s-1 ).Consistent with the density functional theory (DFT) calculations, the real-time kinetic simulation reveals that the conversion from O* to OOH* is the rate-determining step on the active sites of MIL-53(Fe)-2OH |
|---|---|
| Beschreibung: | Date Completed 24.02.2023 Date Revised 24.02.2023 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
| ISSN: | 1521-4095 |
| DOI: | 10.1002/adma.202208904 |