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Title: The direct partial oxidation of methane to liquid hydrocarbons over HZSM-5 zeolite catalyst

Abstract

The direct partial oxidation (DPO) of CH{sub 4} with O{sub 2} in the presence of a C{sub 3} additive over HZSM-5 zeolite catalyst at 960 psig produced C{sub 5}{sup +} liquid hydrocarbons at the expense of the initially formed CH{sub 3}OH. Previous experiments with pure CH{sub 4} and O{sub 2} feed and with a sand-packed reactor conclusively showed the need for both the C{sub 3} additive and the zeolite in the system to produce C{sub 5}{sup +} liquids. Evidence of CH{sub 4} incorporation into the liquid products was given by selectivity calculations which indicated the C{sub 3} alone could not account for the C{sub 5}{sup +} hydrocarbons. CH{sub 4} incorporation has been conclusively confirmed by mass spectral analyses of tetramethylbenzene produced in a run with {sup 13}CH{sub 4} under identical conditions which show significant {sup 13}C enrichment in the C{sub 9}H{sub 11}{sup +} and C{sub 6}H{sub 5}{sup +} fragments. While CH{sub 4} undergoes DPO to CH{sub 3}OH in the system, two possible reaction mechanisms can explain the role of C{sub 3}; one involves C{sub 3} aromatization followed by aromatics alkylation with CH{sub 3}OH. Studies on this system with HZSM-5 catalysts having varying Al contents indicate a sensitivity to zeolite aciditymore » except at high Al concentrations.« less

Authors:
; ; ; ;  [1]
  1. (Mobil Research and Development Corp., Princeton, NJ (United States))
Publication Date:
OSTI Identifier:
7150471
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Catalysis; (United States); Journal Volume: 136:2
Country of Publication:
United States
Language:
English
Subject:
03 NATURAL GAS; 10 SYNTHETIC FUELS; METHANE; CATALYTIC REFORMING; OXIDATION; ZEOLITES; CATALYTIC EFFECTS; ADDITIVES; ALKYLATED AROMATICS; AROMATIZATION; CARBON 13; CHEMICAL REACTION KINETICS; FORMALDEHYDE; GASOLINE; METHANOL; MOLECULAR WEIGHT; NATURAL GAS; SYNTHESIS; ALCOHOLS; ALDEHYDES; ALKANES; AROMATICS; CARBON ISOTOPES; CHEMICAL REACTIONS; ENERGY SOURCES; EVEN-ODD NUCLEI; FLUIDS; FOSSIL FUELS; FUEL GAS; FUELS; GAS FUELS; GASES; HYDROCARBONS; HYDROXY COMPOUNDS; INORGANIC ION EXCHANGERS; ION EXCHANGE MATERIALS; ISOTOPES; KINETICS; LIGHT NUCLEI; LIQUID FUELS; MATERIALS; MINERALS; NUCLEI; ORGANIC COMPOUNDS; PETROLEUM PRODUCTS; REACTION KINETICS; REFORMER PROCESSES; SILICATE MINERALS; STABLE ISOTOPES; 030300* - Natural Gas- Drilling, Production, & Processing; 100200 - Synthetic Fuels- Production- (1990-)

Citation Formats

Han, S., Martenak, D.J., Palermo, R.E., Pearson, J.A., and Walsh, D.E. The direct partial oxidation of methane to liquid hydrocarbons over HZSM-5 zeolite catalyst. United States: N. p., 1992. Web. doi:10.1016/0021-9517(92)90087-X.
Han, S., Martenak, D.J., Palermo, R.E., Pearson, J.A., & Walsh, D.E. The direct partial oxidation of methane to liquid hydrocarbons over HZSM-5 zeolite catalyst. United States. doi:10.1016/0021-9517(92)90087-X.
Han, S., Martenak, D.J., Palermo, R.E., Pearson, J.A., and Walsh, D.E. Sat . "The direct partial oxidation of methane to liquid hydrocarbons over HZSM-5 zeolite catalyst". United States. doi:10.1016/0021-9517(92)90087-X.
@article{osti_7150471,
title = {The direct partial oxidation of methane to liquid hydrocarbons over HZSM-5 zeolite catalyst},
author = {Han, S. and Martenak, D.J. and Palermo, R.E. and Pearson, J.A. and Walsh, D.E.},
abstractNote = {The direct partial oxidation (DPO) of CH{sub 4} with O{sub 2} in the presence of a C{sub 3} additive over HZSM-5 zeolite catalyst at 960 psig produced C{sub 5}{sup +} liquid hydrocarbons at the expense of the initially formed CH{sub 3}OH. Previous experiments with pure CH{sub 4} and O{sub 2} feed and with a sand-packed reactor conclusively showed the need for both the C{sub 3} additive and the zeolite in the system to produce C{sub 5}{sup +} liquids. Evidence of CH{sub 4} incorporation into the liquid products was given by selectivity calculations which indicated the C{sub 3} alone could not account for the C{sub 5}{sup +} hydrocarbons. CH{sub 4} incorporation has been conclusively confirmed by mass spectral analyses of tetramethylbenzene produced in a run with {sup 13}CH{sub 4} under identical conditions which show significant {sup 13}C enrichment in the C{sub 9}H{sub 11}{sup +} and C{sub 6}H{sub 5}{sup +} fragments. While CH{sub 4} undergoes DPO to CH{sub 3}OH in the system, two possible reaction mechanisms can explain the role of C{sub 3}; one involves C{sub 3} aromatization followed by aromatics alkylation with CH{sub 3}OH. Studies on this system with HZSM-5 catalysts having varying Al contents indicate a sensitivity to zeolite acidity except at high Al concentrations.},
doi = {10.1016/0021-9517(92)90087-X},
journal = {Journal of Catalysis; (United States)},
number = ,
volume = 136:2,
place = {United States},
year = {Sat Aug 01 00:00:00 EDT 1992},
month = {Sat Aug 01 00:00:00 EDT 1992}
}