摘要:
Arene hydrogenation activities of catalysts prepared by:tethering. Rh(COD)[H2NCH2CH2NHCH2CH2CH2Si(OCH3)(3)](X) on the silica support of the bimetal catalyst Au:Pb-SiO2 were studied under the mild conditions of 40 degrees C and 1 atm H-2 pressure. The most active catalyst PF6-Rh(N-N)/Au:Pd-SiO2, with the weakly coordinating PF6 anion, remains highly active for toluene hydrogenation through at least three catalytic cycles involving 2900 mol H-2/mol Rh turnovers over a 19-h period. As compared with the activity of the Pd-supported catalyst PF6-Rh(N-N)/Pd-SiO2, the catalysts with added Au are less active only by a factor of two. But the activity depends strongly on the Pd and Rh complex loadings, Although the detailed functioning of these TCSM catalysts (tethered complex on a supported metal) is not known, a mechanism that is consistent with the results involves dissociative adsorption of H-2 On the supported Pd. The hydrogen spills over onto the silica surface where the Rh complex uses it to hydrogenate the arene substrate. (C) 1999 Elsevier Science B.V. All rights reserved.