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• W2894226952 endingPage "3630" @default.
• W2894226952 startingPage "3619" @default.
• W2894226952 abstract "A series of cationic palladium complexes [Pd(N∧N′)Me(NCMe)]+ was synthesized, comprising three different N∧N′-bidentate coordinating pyridyl–pyridylidene amide (PYA) ligands with different electronic and structural properties depending on the PYA position (o-, m-, and p-PYA). Structural investigation in solution revealed cis/trans isomeric ratios that correlate with the donor properties of the PYA ligand, with the highest cis ratios for the complex having the most donating o-PYA ligand and lowest ratios for that with the weakest donor p-PYA system. The catalytic activity of the cationic complexes [Pd(N∧N′)Me(NCMe)]+ in alkene insertion and dimerization showed a strong correlation with the ligand setting. While complexes bearing more electron donating m- and o-PYA ligands produced butenes within 60 and 30 min, respectively, the p-PYA complex was much slower and only reached 50% conversion of ethylene within 2 h. Likewise, insertion of methyl acrylate as a polar monomer was more efficient with stronger donor PYA units, reaching a 32% ratio of methyl acrylate vs ethylene insertion. Mechanistic investigations about the ethylene insertion allowed detection, for the first time, by NMR spectroscopy both cis- and trans-Pd-ethyl intermediates and, furthermore, revealed a trans to cis isomerization of the Pd-ethyl resting state as the rate-limiting step for inducing ethylene conversion. These PYA palladium complexes induce rapid double-bond isomerization of terminal to internal alkenes through a chain-walking process, which prevents both polymerization and also the conversion of higher olefins, leading selectively to ethylene dimerization." @default.
• W2894226952 created "2018-10-05" @default.
• W2894226952 creator A5027700098 @default.
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• W2894226952 date "2018-09-24" @default.
• W2894226952 modified "2023-10-10" @default.
• W2894226952 title "Olefin Dimerization and Isomerization Catalyzed by Pyridylidene Amide Palladium Complexes" @default.
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• W2894226952 doi "https://doi.org/10.1021/acs.organomet.8b00422" @default.
• W2894226952 hasPublicationYear "2018" @default.
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