Direct catalytic conversion of methane and light hydrocarbon gases. Quarterly report No. 7, April 16, 1988--July 15, 1988

The goal of this research is to develop catalysts that directly convert methane and light hydrocarbons to intermediates that later can be converted to either liquid fuels or value-added chemicals, as economics dictate. During this reporting period, much of our effort focused on investigating the stability of the methane reforming catalysts (Task 2) with respect to storage time. Many of these catalysts demonstrated lessened activity when they were reexamined up to 18 months after they ere first synthesized and tested. We also synthesized and tested two new phthalocyanines supported on magnesia (MgO) for examination in the methane oxidation reaction. We reexamined many of the hexaruthenium and tetraruthenium clusters which had been supported on zeolite Y, zeolite 5A, alumina or magnesia. These reexaminations were conducted at relatively slow flow rates (15 ml/min), since previous studies had shown that the lower flow rates maximized the conversion of methane in this reaction. In every case, the catalyst exhibited diminished activity compared to the earlier runs. In addition, the selectivity of the catalysts changed as well; relatively less C{sub 2} and no C{sub 6} was observed in the reactions conducted during this reporting period. In the previous technical report we reported that palladium tetrasulfophthalocyanine (PDTSPC) supported on MgO exhibited exceptional activity in the methane oxidation reaction; it produced ethane at much lower temperatures than previously reported in the literature. We synthesized two close analogues of this compound, one with a different metal (nickel) from the same family as palladium, and the other with a different substituent (carboxylic acid rather than sulfonic acid) on the phthalocyanine ring. Both of these complexes were supported on magnesia, and tested for activity. The nickel complex displayed some activity, producing only carbon dioxide and water