Abstract
The catalytic performance in ethylene hydroformylation over SiO 2, MgO, and carbon-supported Ru, Ru-Co, Ru-Mn, Ru-Cr, and Co carbonyl cluster-derived catalysts has been investigated, and it was found that the catalysts derived from Ru monometallic and Ru-Co bimetallic carbonyl clusters are active in ethylene hydroformylation. The presence of Co atoms in Ru-Co carbonyl clusters led to a remarkable increase in the rate of product formation, especially for oxygenates. The Ru-Mn bimetallic carbonyl cluster-derived catalyst showed similar conversion, but it exhibited poor activity and selectivity for oxygenates as compared with catalysts derived from Ru 6C(CO) 17. In contrast to the Ru 6C(CO) 17 carbonyl cluster-derived catalyst, the Ru-Cr bimetallic carbonyl cluster-derived catalyst exhibited very low activity and selectivity for ethane and oxygenates, indicating that the Cr sites in Ru-Cr bimetallic carbonyl cluster-derived catalyst have a poisoning effect on ethylene hydroformylation. The nature of support has been shown to have a large influence on the catalytic activity and selectivity of the resulting catalyst. The effect of Co promotion in Ru-Co carbonyl clusters on silica and carbon was much stronger than that on MgO. The nature of these Ru-Co/SiO 2 catalyts has been investigated by infrared and X-ray photoelectron spectroscopes. The IR spectra of CO on reduced Ru-Co/SiO 2 catalysts prepared from Ru-Co bimetallic carbonyl clusters exhibited bands at 1684 cm −1. The reaction of CO and H 2 with Ru-Co/SiO 2 catalysts showed a band at 1584 cm −1. In situ IR spectra of the reaction of CO + H 2 + C 2H 4 on these reduced Ru-Co/SiO 2 catalysts exhibited bands at 1585 and 1555 cm −1 shifting to 1540 and 1520 cm −1 by 13CO isotopic effect, which are strongly related to the activity and selectivity for propanol and propaldehyde in ethylene hydroformylation.
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