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Metallocorroles involving 5d transition metals are currently of interest as near-IR phosphors and as photosensitizers for oxygen sensing and photodynamic therapy. Their syntheses, however, are often bedeviled by capricious and low-yielding protocols. Against this backdrop, we describe rhenium-imido corroles, a new class of 5d metallocorroles, synthesized simply and in respectable (∼30%) yields via the interaction of a free-base corrole, Re2(CO)10, K2CO3, and aniline in 1,2,4-trichlorobenzene at ∼190 °C in a sealed vial under strict anaerobic conditions. The generality of the method was shown by the synthesis of six derivatives, including those derived from meso-tris(pentafluorophenyl)corrole, H3[TPFPC], and five different meso-tris(p-X-phenyl)corroles, H3[TpXPC], where X = CF3, F, H, CH3, OCH3. Single-crystal X-ray structures obtained for two of the complexes, Re[TpFPC](NPh) and Re[TpCF3PC](NPh), revealed relatively unstrained equatorial Re-N distances of ∼2.00 Å, a ∼ 0.7-Å displacement of the Re from the mean plane of the corrole nitrogens, and an Re-Nimido distance of ∼1.72 Å. Details of the corrole skeletal bond distances, diamagnetic 1H NMR spectra, relatively substituent-independent Soret maxima, and electrochemical HOMO-LUMO gaps of ∼2.2 V all indicated an innocent corrole macrocycle. Surprisingly, unlike several other classes of 5d metallocorroles, the Re-imido complexes proved nonemissive in solution at room temperature and also failed to sensitize singlet oxygen formation, indicating rapid radiationless deactivation of the triplet state, presumably via the rapidly rotating axial phenyl group. By analogy with other metal-oxo and -imido corroles, we remain hopeful that the Re-imido group will prove amenable to further elaboration and thereby contribute to the development of a somewhat challenging area of coordination chemistry.
Macromolecular and materials chemistry, VDP::Mathematics and natural science: 400::Chemistry: 440, 540, Inorganic Chemistry, VDP::Matematikk og Naturvitenskap: 400::Kjemi: 440, Chemical Sciences, Inorganic & Nuclear Chemistry, Other Chemical Sciences, Inorganic chemistry, Physical Chemistry (incl. Structural)
Macromolecular and materials chemistry, VDP::Mathematics and natural science: 400::Chemistry: 440, 540, Inorganic Chemistry, VDP::Matematikk og Naturvitenskap: 400::Kjemi: 440, Chemical Sciences, Inorganic & Nuclear Chemistry, Other Chemical Sciences, Inorganic chemistry, Physical Chemistry (incl. Structural)
citations This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically). | 19 | |
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impulse This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network. | Top 10% |