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A study was made of the dehydrogenation of n‐butane over a commercial chromia‐alumina catalyst. Dehydrogenation runs were performed at 500°C. and space velocity of 34,000 hr−1 over a range of butane partial pressures from 0.06 to 1.80 atm. Conversions were differential, averaging about 3% (with a maximum of 6% ) of the input butane. Reaction was found to be 0.75 order in butane partial pressure. Thermodynamic equilibrium was attained among the products, which were 1‐butene, cis‐2‐butene, and trans‐2‐butene. The method of Yang and Hougen showed dehydrogenation to be surface reaction controlled at a confidence level of 91%. This conclusion agrees with that of a previous study by Dodd and Watson.
A study was made of the dehydrogenation of n‐butane over a commercial chromia‐alumina catalyst. Dehydrogenation runs were performed at 500°C. and space velocity of 34,000 hr−1 over a range of butane partial pressures from 0.06 to 1.80 atm. Conversions were differential, averaging about 3% (with a maximum of 6% ) of the input butane. Reaction was found to be 0.75 order in butane partial pressure. Thermodynamic equilibrium was attained among the products, which were 1‐butene, cis‐2‐butene, and trans‐2‐butene. The method of Yang and Hougen showed dehydrogenation to be surface reaction controlled at a confidence level of 91%. This conclusion agrees with that of a previous study by Dodd and Watson.
Pulsed microcatalytic reactors have found extensive application in the petroleum and chemical industries where rapid catalyst screening and evaluation are demanded. Automated, continuous‐operation test units allow the accumulation of considerable amounts of data in a minimum of time. The technique is also useful in research where the small pulse size enables one to study “initial” interactions between surface and reactants. In this way, information about many kinetic parameters, such as intrinsic reaction rates, orders, poisoning effects, and catalyst deactivation, can be obtained. Both stable and radioactive isotopic tracers may be used economically in microcatalytic reactors to provide significant mechanistic information which cannot be obtained conveniently by other methods. For example, one can explore the chemical nature and number of active sites, as well as the fate of individual atoms and molecules as they interact with the catalyst. Although the technique may be applied to both “simple” and complex catalytic reaction systems, the discussion will be limited to a review of data obtained from (1) “unimolecular” reactions such as cyclopropane and butene isomerization and cumene dealkylation over the mixed oxides silica‐alumina, silica‐magnesia, and zeolites and (2) “bimolecular” reactions such as ethylene hydrogenation over alumina. Some of the limitations of microcatalytic reactors will also be given.
The acidity of MoO3·γ‐Al2O3, MoO3·SiO2, MoO3·SiO2·Al2O3 systems has been determined by measuring the heat of immersion in pyridine; a non‐monotonic variation with the MoO3 percentage has been observed in the range from 0 ‐ 25 wt% MoO3. The extremes are: 4, 8*, 15 and 25* wt % MoO3 on γ‐A2O3; 3,4*, 7, 13*, 16 and 23* wt % MoO3 on SiO2; 1*, 2, 8* and 25 wt % MoO3 on SiO2·Al2O3, where asterisks denote maxima. For the MoO3·Al2O3 and MoO3·SiO2 systems the activity for double‐bond isomerization of 1‐butene has been measured in the temperature range of 200‐245° and apparent activation energies ΔEa have been derived. As a function of the composition, ΔEa shows a minimum for the 14 wt% MoO3·SiO2, a weak maximum (16 wt%) and a steep minimum (8 wt%) for MoO3·Al2O3 catalysts. The selectivity of the isomerisation reaction has been discussed in terms of surface structure and acidity. It is concluded that the formation of various catalytic species rather than the variation of acidity or the deposition of carbonaceous residues accounts for the selectivity of MoO3·Al2O3 and MoO3·SiO2 catalysts towards isomerization of 1‐butene to cis‐ and trans‐2‐butene and therefore for the variation of the apparent activation energy with composition.
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