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Details van artikel 29 van 86 gevonden artikelen
| Titel: |
New media in homogeneous catalysis: wet sodium or tetrabutylammonium hydrogensulfate salts for reppe syntheses catalyzed by a ru(ii) carbonyl complex |
| Auteur: |
Pardey, Alvaro J. Rivas, Angel B. Longo, Clementina Funaioli, Tiziana Fachinetti, Giuseppe |
| Verschenen in: |
Journal of coordination chemistry |
| Paginering: | Jaargang 57 (2004) nr. 10 pagina's 871-882 |
| Jaar: |
2004-07-10 |
| Inhoud: |
The ruthenium(II) complex fac-[Ru(CO)2(H2O)3(C(O)C2H5)][CF3SO3] dissolved in aqueous tetrabutylammonium hydrogensulfate ([(CH3(CH2)3)4N][HSO4]) or sodium hydrogensulfate (NaHSO4) catalyzes the hydrocarboxylation of ethylene to propionic acid and additionally produces minor amounts of hydrocarbonylation products (diethyl ketone and propanal), under water-gas shift reaction conditions. This system is stable with a selectivity of 90% to propionic acid for high ethylene conversion. A turnover frequency of propionic acid, TOF(C2H5CO2H)/24 h = 5 × 103 (TOF (C2H5CO2H) = ([(moles of C2H5CO2H)/(moles of Ru) × rt)] × 24 h) was achieved for Ru = 7.45 × 10-4 mol, [(CH3(CH2)3)4N][HSO4] = 80 g (2.36 × 10-2 mol); H2O = 40 g (2.22 mol); CO = C2H4 = 20 g (total pressure = 88 atm); T = 150°C by a reaction time (rt) of 2.87 h. The countercation (sodium or tetrabutylammonium), the ruthenium concentration and the hydrogensulfate/H2O ratio of the medium affect the catalytic reaction. A nonlinear dependence on total ruthenium concentration was shown. The data are discussed in terms of a potential catalytic cycle. Formation of propionic acid comes from hydrolysis, and formation of diethyl ketone and propanal comes from hydrogenolysis of the Ru-ketyl and Ru-acyl complexes, respectively. |
| Uitgever: |
Taylor & Francis |
| Bronbestand: |
Elektronische Wetenschappelijke Tijdschriften |
Details van artikel 29 van 86 gevonden artikelen
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