Direct synthesis of higher alcohols by catalytic hydrogenation of carbon oxides
Three objectives of this research project were : 1) to derive a catalyst and operating conditions which would result in the conversion of synthesis gas to as near 100% methanol as possible with no by-products such as methane, dimethyl-ether, or higher alcohols; 2) to derive catalysts and conditions whereby CO, H/sub 2/, and optionally CO/sub 2/ would be converted to crude alcohols containing 65 to 75% methanol and 25 to 35% higher alcohols (C/sub 2/ to C/sub 6/) while reacting 5% or less of the CO to CH/sub 4/ and other hydrocarbons; and 3) to attain this product at a rate of 0.5 ml/hr/(ml catalyst). The crucial factors in the catalyst composition and processing conditions are as follows: (1) A relatively high proportion of Cu (4 molar) and Mn (3 molar), (2) Zn equivalent to approximately 25% (molar) of the Cu or Mn, (3) Co equivalent to approximately 0.1% to 0.6% (molar) of the Cu, (4) A stabilizer-promoter which consists of Cr/sub 2/O/sub 3/ and optionally oxides of Al, Zr, Mg (10% and 5% by weight) respectively, (5) A moderator, approximately 4% (by weight) of the total catalyst employed, consisting of Rb, Cs, or K, or some combination of these, (6) Preferred operating conditions of 2500 psi pressure, 40,000 hr/sup -1/ space velocity, approximately 400/sup 0/C, and an almost stoichiometric feed-gas composition somewhat rich in CO, which is a unique departure from normal operation conditions. The catalyst preparation procedure is critical and is reported in detail. The catalyst has also been physically characterized in the used and unused conditions, and these observations are also reported. The mechanistic implications of the results of this study are discussed. Pathways involving the crossed aldol condensation (for the formation of primary aldehydes and alcohols) and the Claisen condensation (for the generation of ketones and secondary alcohols) for the higher alcohols synthesis are proposed.
- Research Organization:
- Delaware Univ., Newark (USA)
- OSTI ID:
- 7015439
- Resource Relation:
- Other Information: Thesis (Ph. D.)
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
ALCOHOLS
CHEMICAL PREPARATION
ALUMINIUM OXIDES
CATALYTIC EFFECTS
CARBON DIOXIDE
CHEMICAL REACTIONS
CARBON MONOXIDE
CESIUM
CHROMIUM OXIDES
COBALT
COPPER
HYDROGEN
MAGNESIUM OXIDES
MANGANESE
POTASSIUM
RUBIDIUM
SYNTHESIS GAS
ZINC
ZIRCONIUM OXIDES
CATALYSIS
ALKALI METALS
ALKALINE EARTH METAL COMPOUNDS
ALUMINIUM COMPOUNDS
CARBON COMPOUNDS
CARBON OXIDES
CHALCOGENIDES
CHROMIUM COMPOUNDS
ELEMENTS
FLUIDS
GASES
HYDROXY COMPOUNDS
MAGNESIUM COMPOUNDS
METALS
NONMETALS
ORGANIC COMPOUNDS
OXIDES
OXYGEN COMPOUNDS
SYNTHESIS
TRANSITION ELEMENT COMPOUNDS
TRANSITION ELEMENTS
ZIRCONIUM COMPOUNDS
090221* - Alcohol Fuels- Chemical Synthesis- (1976-1989)