Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 143, Issue 38, Pages 15661-15673Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c06081
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Funding
- Fonds National pour la Recherche Scientifique (F.R.S.-FNRS)
- Charge de Recherches individual fellowship
- National Science Foundation [DGE-1650116]
- U.S. Department of Energy, Office of Basic Energy Sciences, Office of Science [DE-SC0021173]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences Biosciences [DE-SC0012704]
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Efficient excited-state electron transfer was achieved between an iron(III) photosensitizer and organic electron donors under green light irradiation, using a long-lived and luminescent ligand-to-metal charge-transfer (LMCT) excited state iron photosensitizer. The catalyst demonstrated yields exceeding 90% in a benchmark dehalogenation reaction, with enhanced stability compared to a typical photosensitizer. The initial catalytic step involved electron transfer from an amine to the photoexcited iron sensitizer, shown to occur with a large cage-escape yield, indicating potential advantages of Fe(III) photosensitizers in reductive electron transfer.
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.
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