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Superacid catalysis of light hydrocarbon conversion. Sixth quarterly report, January 1, 1995--March 31, 1995

Technical Report ·
DOI:https://doi.org/10.2172/95596· OSTI ID:95596
 [1]
  1. California Univ., Davis, CA (United States). Dept. of Chemical Engineering and Materials Science

Iron- and Manganese-promoted sulfated zirconia is a catalyst for the conversion of propane, but the rate of conversion of propane is much less than the rate of conversion of butane. Whereas this catalyst appears to be a good candidate for practical, industrial conversion of butane, it appears to lack sufficient activity for practical conversion of propane. Perhaps more active catalysts will be useful for propane conversion. The propane conversion data reported here provide excellent insights into the chemistry of the catalytic conversions; they are consistent with the inference that the catalyst is a superacid and that the chemistry is analogous to. that determined in superacid solutions by G.A. Olah, who was awarded the most recent Nobel Prize in chemistry for his work. The catalyst was tested for conversion of propane at 1 bar, 200--300{degrees}C and propane partial pressures in the range of 0.01--0.05 bar. At 250{degrees}C, catalysis was demonstrated, as the number of propane molecules converted was at least 1 per sulfate group after 16 days of operation in a continues flow reactor. Propane was converted in high yield to butanes, but the conversions were low, for example being only a fraction of a percent at a space velocity of 9.1 {times} 10{sup {minus}7} mol(g of catalysis {center_dot} s) and 250{degrees}C. Coke formation was rapid. The observation of butanes, pentanes, and methane as products is consistent with Olah superacid chemistry, whereby propane is first protonated by a very strong acid to form a carbonium ion. The carbonium ion then decomposes into methane and an ethyl cation which undergoes oligocondensation reactions with propane to form higher molecular weight alkanes. The results are consistent with the identification of iron- and manganese-promoted sulfated zirconia as a superacid.

Research Organization:
Delaware Univ., Newark, DE (United States); California Univ., Davis, CA (United States). Dept. of Chemical Engineering and Materials Science
Sponsoring Organization:
USDOE, Washington, DC (United States)
DOE Contract Number:
AC22-93PC92116
OSTI ID:
95596
Report Number(s):
DOE/PC/92116--T6; ON: DE95016276
Country of Publication:
United States
Language:
English