Fundamental Studies of the Mechanism of Catalytic Reactions with Catalysts Effective in the Gasification of Carbon Solids and the Oxidative Coupling of Methane . Quarterly Report PDF Download
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Languages : en
Pages : 54
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Work on catalytic steam gasification with chars and coals will be extended from atmospheric to elevated pressures using the newly built pressure unit. The novel finding that coking of petroleum in the presence of small amounts of caustic greatly improves the gasification rates and characteristics of the coke will be extended to chars; in the oxidative coupling of methane over ternary catalysts, emphasis will be placed on low temperature coupling and on the oxidative production of syngas from methane at low temperature. Experimental work will continue on the synthesis of the mixed catalyst, and they will be characterized by a number of techniques, including elemental analyses, x-ray diffraction, and surface area determination.
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Pages : 17
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Research continued on the study of catalysts and membrane materials involved in the oxidative coupling of methane and coal gasification processes. Membranes studied and fabricated included Sr-Zr-Y-O, Sr-Zr-Y, and Sr-Ce-Y-O systems.
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Languages : en
Pages : 31
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This report describes research on the oxidative coupling of methane and catalysts involved in coal gasification. Topics include methane pyrolysis and catalysts, and magnetic properties of the coal gasification catalyst Ca-Ni-K-O system.
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Languages : en
Pages : 17
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Work will continue on the oxidative coupling reaction of methane over ternary oxide catalysts to produce C2, C3 and C4 hydrocarbons and Particularly Olefins with high selectivity. The work which has shown that close to 100% selectivity can be obtained has received wide attention and has resulted in collaborative efforts with industry (CRADA) towards the development of a commercial process. An immediate purpose of additional work is to increase the conversion without diminishing the extremely high selectivity of the reaction and also to permit operation at higher space velocity to reduce equipment size. The mechanism of this reaction is not understood and much additional work is needed to explain the role of carbon formation and of water as intermediates in the reaction and to investigate whether carbon oxides are intermediates. It has been found that oxides other than calcium-nickel-potassium oxides can be useful catalysts for this reaction in the presence of steam and at relatively low temperatures and long contact times. Better definition of the class of binary metal oxides is required and better catalyst characterization is needed to ensure reproducibility Of catalyst preparation and operational results. Pretreatment of the catalyst should be shortened and higher space velocities must be obtained. Close collaboration with Orion ACT is required to advance the project toward the pilot plant stage. In the area of coal and char catalytic steam gasification, the large volume of data obtained at atmospheric pressure will be extended to operations at higher pressures.
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Languages : en
Pages : 10
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The synthesis of ethane and ethylene from methane and oxygen will be carried out in novel hydrogen transport inorganic membranes and in cyclic reactors in order to prevent undesirable secondary reactions of C2 molecules to CO and CO2. Neither inorganic membrane reactors nor cyclic tubular reactors are presently used in commercial processes. Their application to catalytic reactions represents a novel application of engineering and solid-state chemistry concepts to catalytic reactions. Our approach combines high temperature membrane and cyclic experimental reactors, synthesis and characterization of thin membrane films and of high surface area catalysts, and detailed models of complex gas phase and surface reactions involved in oxidative coupling. We anticipate that this approach will lead to novel reactors for carrying our kinetic-controlled sequential reactions, such as the oxidative coupling of methane. Careful spectrographic and wet chemical analyses of fresh and silent catalysts have shown considerable differences which have permitted conclusions as to the source of deactivation. Our activities in the first quarter FYI 995 have focused on the synthesis, structural characterization, and catalytic evaluation of membrane films, disks, and reactors. We have also continued to exploit reaction-transport models to predict the performance of membrane, cyclic, and recycle reactors in the oxidative coupling of methane.
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Languages : en
Pages : 20
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The last quarterly report (LBL-33769) summarized results obtained with ternary catalysts; e.g., K-Ca-Ni oxide and K-Ca-Co oxide. It was also shown that chars prepared in e presence of NAOH were more easily gasified than the base char, even if the chars were washed to remove all residual free NAOH. During the present report quarter, three variables were investigated: (1) The effect of varying the atomic ratio of different catalyst components (alkali vs. transition metal); (2) The effect of steam partial pressure and of temperature on the reaction; (3) Determination of activation energy of the reaction over K-Ca-Co oxide. It was also found that if the water (steam) used for gasification contains a small amount of NAOH, gasification rates are greatly improved. Figure 1 shows that the gasification rate improves with increasing Co content of the catalyst, though the differences between different Co contents are relatively small. A very similar effect was observed for different concentrations of Fe{sup 3+} in KCa-Fe oxide catalysts. Figure 2 presents conversion vs. time plots for gasification of an Ill {number_sign}6 char (which had been charred in the presence of 0.5% caustic) over a K-Ca-Co oxide catalyst at four temperatures. As expected the gasification rate increases with temperature, although there is little difference between our standard 640°C and 680°C. Figure 3 investigates the effect of partial pressure of water on the conversion using an Ill {number_sign}6 char (prepared in the presence of 0.5% caustic) and a K-Ca-Co oxide catalyst at 640°C. There is an improvement in rate with increasing water partial pressure.
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Languages : en
Pages : 14
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Work continued on the development of catalysts for the steam gasification of chars and for the oxidative coupling of methane. Testing of the catalysts Ni-Ca-K-oxides and Co-Ca-K-oxides are described for gasification research; results of the testing of a Co-Mg-oxide catalysts for methane conversion are also described.
