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Design of a high activity and selectivity alcohol catalyst

Technical Report ·
DOI:https://doi.org/10.2172/6776377· OSTI ID:6776377
Efforts to synthesize bimetallic cluster-derived Rh-Mo catalysts for CO and CO[sub 2] hydrogenation to preferentially produce oxygenates. The rhodium-molybdenum cluster, (PPh[sub 3])[sub 2]RhMO(CO)([mu]-CO)[sub 2]Cp, was employed as a precursor to alumina- and silica-supported catalysts which were in CO hydrogenation. When compared to catalysts made from the distinct organometallic complexes, RhH(CO)(PPh[sub 3])[sub 3] and [MO(CO)[sub 3]Cp][sub 2], the catalysts derived from a binuclear precursor show higher activities for CO hydrogenation and superior selectivities towards oxygenates, namely, methanol, dimethyl ether and ethanol. Their product distributions depend on the support. Fourier transform infrared spectroscopy studies indicate that CO chemisorbs on cluster-derived catalysts as gem-dicarbonyls while it is chemisorbed only in the linear-carbonyl configuration on catalysts made from separate rhodium and molybdenum complexes. The particular oxygenate selectivity of the cluster-derived catalysts may be correlated to the strong electronic interaction between Rh and Mo. Carbon dioxide hydrogenation has also been carried out on the catalysts mentioned above. Again, the cluster-derived catalysts show higher oxygenate selectivities. Finally, the catalysts were studied with regard to both CO and CO[sub 2] hydrogenation kinetics, apparent activation energies inferred.
Research Organization:
Delaware Univ., Newark, DE (United States). Center for Catalytic Science and Technology
Sponsoring Organization:
DOE; USDOE, Washington, DC (United States)
DOE Contract Number:
FG22-90PC90291
OSTI ID:
6776377
Report Number(s):
DOE/PC/90291-T10; ON: DE93008103
Country of Publication:
United States
Language:
English