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• W4384007966 endingPage "2024" @default.
• W4384007966 startingPage "2007" @default.
• W4384007966 abstract "A series of CS-symmetric (aryl,alkyl)-substituted pyridine(dimine) iron methyl (CyARPDI)FeCH3 complexes have been prepared, characterized, and evaluated as precatalysts for the [2+2]-cycloaddition of butadiene and ethylene. Mixtures of vinylcyclobutane and (Z)-hexa-1,4-diene were observed in each case. By comparison, C2v-symmetric, arylated (PDI) iron catalysts are exclusively selective for reversible [2+2]-cycloaddition to yield vinylcyclobutane. The alteration in the chemoselectivity of the catalytic reaction was investigated through a combination of precatalyst stability studies, identification of catalytic resting state(s), and 2H and 13C isotopic labeling experiments. While replacement of an aryl-imine substituent with an N-alkyl group decreases the stability of the formally iron(0) dinitrogen and butadiene complexes, two diamagnetic metallacycles were identified as catalyst resting states. Deuterium labeling and NOESY/EXSY NMR experiments support 1,4-hexadiene arising from catalytic hydrovinylation involving reversible oxidative cyclization leading to accessible cis-metallacycle. Cyclobutane formation proceeds by irreversible C(sp3)–C(sp3) bond-forming reductive elimination from a trans-metallacycle. These studies provide key mechanistic understanding into the high selectivity of bis(arylated) pyridine(diimine) iron catalysts for [2+2]-cycloaddition, unique, thus far, to this class of iron catalysts." @default.
• W4384007966 created "2023-07-13" @default.
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• W4384007966 date "2023-07-12" @default.
• W4384007966 modified "2023-09-25" @default.
• W4384007966 title "<i>C</i>_S-Symmetric Pyridine(diimine) Iron Methyl Complexes for Catalytic [2+2] Cycloaddition and Hydrovinylation: Metallacycle Geometry Determines Selectivity" @default.
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• W4384007966 doi "https://doi.org/10.1021/jacsau.3c00229" @default.
• W4384007966 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/37502155" @default.
• W4384007966 hasPublicationYear "2023" @default.
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