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• W4387132141 abstract "The interconversion rates of the syn- and anti-isomers of the neutral molybdenum and tungsten imido alkylidene N-heterocyclic carbene (NHC) complexes of the general formula [M(NR)(CHCMe2R′)(NHC)(OR″)2] (M = Mo, W; R = adamantyl, 2,6-Me2-C6H3, 2,6-iPr2–C6H3, 2,6-Cl2–C6H3, 2-tBu-C6H4; NHC = 1,3-diisopropylimidazol-2-ylidene (IiPr), 1,3-dimethylimidazol-2-ylidene (IMe), 1,3-dicyclohexylimidazol-2-ylidene (ICy), and 1,3-dimesitylimidazol-2-ylidene (IMes); R′ = Me, Ph; R″ = CMe(CF3)2, CMe2(CF3), C(CF3)3, C6F5, SO2CF3) and of the cationic complex [Mo(N-2,6-Me2-C6H3)(CHCMe2Ph)(IMes)(SO3CF3)(CD3CN)+ B(3,5-(CF3)2C6H3)4–] were determined by irradiating solutions of the catalysts with 366 nm UV light followed by recording the back-isomerization of the anti- to the syn-isomer. Both the rate of anti to syn and syn to anti interconversion, ka/s and ks/a were found to be orders of magnitude lower than in tetracoordinated, neutral Schrock catalysts of the general formula [Mo(NR)(CHCMe2R′)(OR″)2]. Accordingly, the values for the Gibbs free energy of the transition state, ΔG‡, are significantly higher for both neutral and cationic molybdenum and tungsten imido alkylidene NHC complexes than for Schrock catalysts. NMR investigations strongly suggest that these higher ΔG‡ values are attributable to dissociation of an anionic ligand from a neutral pentacoordinated catalyst that precedes interconversion. As with Schrock catalysts, the anti-isomer proved to be the more reactive isomer, in both ring-opening metathesis polymerization and ring-closing metathesis (RCM) reactions, allowing for higher productivities, expressed as turnover numbers, in RCM." @default.
• W4387132141 created "2023-09-29" @default.
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• W4387132141 date "2023-09-28" @default.
• W4387132141 modified "2023-10-15" @default.
• W4387132141 title "Interconversion Rates and Reactivity of <i>Syn</i>- and <i>Anti</i>-rotamers of Neutral and Cationic Molybdenum and Tungsten Imido Alkylidene <i>N</i>-Heterocyclic Carbene Complexes" @default.
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• W4387132141 doi "https://doi.org/10.1021/acs.organomet.3c00334" @default.
• W4387132141 hasPublicationYear "2023" @default.
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