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The hydrido–amido complex OsH(NHCMe2CMe2NH2)(PPh3)2 (1) catalyzes the base-free hydrogenation of ketones in benzene. Kinetic studies using acetophenone revealed that the system has an induction period, after which the rate of the reaction increases. A constant rate was observed when a critical amount of the product alcohol was added, indicating that the reaction is autocatalytic in 1-phenylethanol. Varying the initial conditions showed that the reaction rate is dependent on hydrogen and catalyst concentration and independent of ketone concentration. Above the critical concentrations of 1-phenylethanol, the reaction rate is independent of alcohol concentration. The rate law for pressures up to 5 atm was found to be rate = d[alcohol]/dt = −d[ketone]/dt = k[Os][H2], with k = 30 mol L−1 s−1 at 293 K and the temperature dependence provided energy of activation parameters. Therefore, the heterolytic splitting of dihydrogen is rate determining under these conditions. Only small kinetic isotope effects were measu...

Alcohol-assisted base-free hydrogenation of acetophenone catalyzed by OsH(NHCMe2CMe2NH2)(PPh3)2

Alcohol-assisted base-free hydrogenation of acetophenone catalyzed by OsH(NHCMe₂CMe₂NH₂)(PPh₃)₂