Mechanistic studies of catalytic methanol synthesis. Final report

Technical Report · Thu Mar 01 04:00:00 EST 1984

DOI:https://doi.org/10.2172/5120585· OSTI ID:5120585

Kung, H. H.

The catalytic methanol production on a Cu-Zn-oxide catalyst was studied at 17 atm and about 200 C in a batch reactor. The initial rate measurement was performed for different CO/sub 2//CO ratios in the feed. The rate was found to increase with increasing CO/sub 2//CO, for a fixed H/sub 2/ partial pressure. This behavior was observed for catalysts at different stages of deactivation, and from 195 to 225 C. Addition of a small amount of water vapor greatly suppressed the rate. When C/sup 18/O/sub 2/ was used in a feed of CO/sub 2/:CO:H/sub 2/ = 3:10:20, the initial rate of production of methanol-/sup 18/O was found to be about half the rate of production of methanol-/sup 16/O. In view of the much lower partial pressure of CO/sub 2/ than CO in the feed, this result suggests that the hydrogenation rate of CO/sub 2/ on a per mole basis is faster than that of CO. This is consistent with the above initial rate data. Production of C/sup 16/O/sup 18/O and C/sup 16/O/sub 2/ were also rapid, which indicated rapid exchange of the lattice oxygen with CO/sub 2/. The production of H/sub 2//sup 18/O was also rapid, being about twice as fast as the methanol production rate. Thus under the conditions of initial rate measurements, the water-gas shift reaction is rapid. The relative rates of hydrogenation of CO/sub 2/ and CO were also determined near chemical equilibrium by the relaxation method. Nonequilibrium thermodynamic theories were applied to describe the relaxation process. The physical meaning of the equilibrium exchange rate for a complex reaction was discovered. A method was developed to mesure the equilibrium exchange rates of the simultaneous reactions in methanol synthesis. 18 references, 4 figures, 3 tables.

• Research Organization: Northwestern Univ., Evanston, IL (USA). Dept. of Chemical Engineering
• DOE Contract Number: FG22-80PC30239
• OSTI ID: 5120585
• Report Number(s): DOE/PC/30239-T4; ON: DE84008380
• Country of Publication: United States
• Language: English

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ALCOHOLS
BETA DECAY RADIOISOTOPES
BETA-MINUS DECAY RADIOISOTOPES
CARBON 16
CARBON 18
CARBON COMPOUNDS
CARBON DIOXIDE
CARBON ISOTOPES
CARBON MONOXIDE
CARBON OXIDES
CATALYTIC EFFECTS
CHALCOGENIDES
CHEMICAL PREPARATION
CHEMICAL REACTION KINETICS
CHEMICAL REACTIONS
COPPER COMPOUNDS
COPPER OXIDES
DATA
EVEN-EVEN NUCLEI
EXPERIMENTAL DATA
HIGH TEMPERATURE
HYDROGENATION
HYDROXY COMPOUNDS
INFORMATION
ISOTOPE APPLICATIONS
ISOTOPES
KINETICS
LIGHT NUCLEI
MEDIUM PRESSURE
METHANOL
NUCLEI
NUMERICAL DATA
ORGANIC COMPOUNDS
OXIDES
OXYGEN 18
OXYGEN COMPOUNDS
OXYGEN ISOTOPES
RADIOISOTOPES
REACTION KINETICS
SECONDS LIVING RADIOISOTOPES
STABLE ISOTOPES
SYNTHESIS
TRACER TECHNIQUES
TRANSITION ELEMENT COMPOUNDS
ZINC COMPOUNDS
ZINC OXIDES