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Investigation of the reduction of carbon monoxide to hydrocarbons and methanol

Thesis/Dissertation ·
OSTI ID:5629904

The current energy shortage has resulted in renewed interest in the synthesis of liquid fuel from coal-derived carbon monoxide and hydrogen. Two important heterogeneous catalytic reactions which can convert carbon monoxide to liquid fuel are the Fischer-Tropsch reaction and the methanol synthesis. This study investigated the mechanism of the Fischer-Tropsch reaction, i.e., the conversion of CO and H/sub 2/ to hydrocarbons in the presence of heterogeneous transition-metal catalysts. The possible synergistic effect of anchoring a homogeneous catalyst onto a heterogeneous methanol catalyst was also examined. The reaction of diazomethane and hydrogen, diluted with an inert gas, on supported transition-metal surfaces such as Co, Ru, Fe, Ni, and Pd was found to produce mainly linear alkanes and alkenes ranging from C/sub 1/ through C/sub 18/ and higher, similar to those found in the Fischer-Tropsch reaction. The distribution of isotopically labelled propene molecules following the reaction of hydrogen and different ratios of /sup 13/CO and /sup 12/CH/sub 2/N/sub 2/ on a cobalt Fischer-Tropsch catalyst was determined. These experimentally observed distributions were consistent with those predicted by Fischer and Tropsch themselves. These results are consistent with a mechanism for the Fischer-Tropsch reaction which involves the formation of carbon-carbon bonds via polymerization of methylene groups. A homogeneous hydrogenation catalyst was covalently anchored to a heterogeneous methanol catalyst in an attempt to generate methanol under milder conditions than are normally required. These attempts were unsuccessful.

OSTI ID:
5629904
Country of Publication:
United States
Language:
English