| Autor: |
Akin Aydogan, Michael D. Turlington, Gerald J. Meyer, Benjamin Elias, Rachel E. Bangle, Alejandro Cadranel, Michael L. Singleton, Emilie Cauet, Daniel T. Conroy, Renato N. Sampaio, Ludovic Troian-Gautier |
| Přispěvatelé: |
UCL - SST/IMCN/MOST - Molecular Chemistry, Materials and Catalysis |
| Jazyk: |
angličtina |
| Rok vydání: |
2021 |
| Předmět: |
|
| Zdroj: |
Journal of the American Chemical Society, Vol. 143, no.38, p. 15661-15673 (2021) |
| Popis: |
Efficient excited-state electron transfer between an iron(III) photosensitizer and organic electron donors was realized with green light irradiation. This advance was enabled by the use of the previously reported iron photosensitizer, [Fe(phtmeimb)2]+ (phtmeimb = {phenyl[tris(3-methyl-imidazolin-2-ylidene)]borate}, that exhibited long-lived and luminescent ligand-to-metal charge-transfer (LMCT) excited states. A benchmark dehalogenation reaction was investigated with yields that exceed 90% and an enhanced stability relative to the prototypical photosensitizer [Ru(bpy)3]2+. The initial catalytic step is electron transfer from an amine to the photoexcited iron sensitizer, which is shown to occur with a large cage-escape yield. For LMCT excited states, this reductive electron transfer is vectorial and may be a general advantage of Fe(III) photosensitizers. In-depth time-resolved spectroscopic methods, including transient absorption characterization from the ultraviolet to the infrared regions, provided a quantitative description of the catalytic mechanism with associated rate constants and yields. |
| Databáze: |
OpenAIRE |
| Externí odkaz: |
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