skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Direct partial oxidation of methane over ZSM-5 catalyst: Metals effects on higher hydrocarbon formation

Abstract

The direct partial oxidation (DPO) of CH[sub 4] with O[sub 2] to higher hydrocarbons, and in particular C[sub 5][sup +] liquids, over metal-containing ZSM-5 catalysts is reported. At 960 psig, 4600 hr[sup [minus]1] GHSV, 7 vol% O[sub 2], and temperatures sufficient for 100% O[sub 2] conversion (440-465[degrees]C), studies with first row transition metals supported on ZSM-5 showed that Cu, Ni, and Zn oxides produced C[sub 5][sup +] liquids (Fe-ZSM-5 produced C[sub 2]-C[sub 4] hydrocarbons) without the need for a feed additive. Co-, Cr-, and Mn-ZSM-5 catalysts under the same conditions produced no higher hydrocarbons. It is believed that of the CH[sub 3]OH formed in the system to higher hydrocarbons over metal-containing ZSM-5 is made possible by two metal functions. Initial trace dehydrogenation of CH[sub 4] (or of minute C[sub 2][sup +] feed components) to olefins provides initiation of the methanol-to-gasoline (MTG) reaction but survival of olefins in the system is a function of the olefin oxidation activity of the metal oxide. Further experimentation using Ga-, Pt-, and Ag-ZSM-5 catalysts was consistent with this hypothesis. Thus, metal-containing ZSM-5 catalysts can produce C[sub 5][sup +] liquids from CH[sub 5] and O[sub 2] if dehydrogenation and oxidation functions of the metal are inmore » balance. 12 refs., 4 tabs.« less

Authors:
; ; ; ;  [1]
  1. (Mobil Research and Development Corp., Princeton, NJ (United States))
Publication Date:
OSTI Identifier:
6798135
Alternate Identifier(s):
OSTI ID: 6798135
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Catalysis; (United States); Journal Volume: 148:1
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 10 SYNTHETIC FUELS; METHANE; OXIDATION; ZEOLITES; CATALYTIC EFFECTS; ALKENES; CATALYST SUPPORTS; CATALYSTS; CHROMIUM; COBALT; COPPER; GALLIUM; HETEROGENEOUS CATALYSIS; MANGANESE; NICKEL; PLATINUM; SILVER; ZINC; ALKANES; CATALYSIS; CHEMICAL REACTIONS; ELEMENTS; HYDROCARBONS; INORGANIC ION EXCHANGERS; ION EXCHANGE MATERIALS; MATERIALS; METALS; MINERALS; ORGANIC COMPOUNDS; PLATINUM METALS; SILICATE MINERALS; TRANSITION ELEMENTS 400201* -- Chemical & Physicochemical Properties; 100200 -- Synthetic Fuels-- Production-- (1990-)

Citation Formats

Han, S., Martenak, D.J., Palermo, R.E., Pearson, J.A., and Walsh, D.E.. Direct partial oxidation of methane over ZSM-5 catalyst: Metals effects on higher hydrocarbon formation. United States: N. p., 1994. Web. doi:10.1006/jcat.1994.1194.
Han, S., Martenak, D.J., Palermo, R.E., Pearson, J.A., & Walsh, D.E.. Direct partial oxidation of methane over ZSM-5 catalyst: Metals effects on higher hydrocarbon formation. United States. doi:10.1006/jcat.1994.1194.
Han, S., Martenak, D.J., Palermo, R.E., Pearson, J.A., and Walsh, D.E.. Fri . "Direct partial oxidation of methane over ZSM-5 catalyst: Metals effects on higher hydrocarbon formation". United States. doi:10.1006/jcat.1994.1194.
@article{osti_6798135,
title = {Direct partial oxidation of methane over ZSM-5 catalyst: Metals effects on higher hydrocarbon formation},
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] to higher hydrocarbons, and in particular C[sub 5][sup +] liquids, over metal-containing ZSM-5 catalysts is reported. At 960 psig, 4600 hr[sup [minus]1] GHSV, 7 vol% O[sub 2], and temperatures sufficient for 100% O[sub 2] conversion (440-465[degrees]C), studies with first row transition metals supported on ZSM-5 showed that Cu, Ni, and Zn oxides produced C[sub 5][sup +] liquids (Fe-ZSM-5 produced C[sub 2]-C[sub 4] hydrocarbons) without the need for a feed additive. Co-, Cr-, and Mn-ZSM-5 catalysts under the same conditions produced no higher hydrocarbons. It is believed that of the CH[sub 3]OH formed in the system to higher hydrocarbons over metal-containing ZSM-5 is made possible by two metal functions. Initial trace dehydrogenation of CH[sub 4] (or of minute C[sub 2][sup +] feed components) to olefins provides initiation of the methanol-to-gasoline (MTG) reaction but survival of olefins in the system is a function of the olefin oxidation activity of the metal oxide. Further experimentation using Ga-, Pt-, and Ag-ZSM-5 catalysts was consistent with this hypothesis. Thus, metal-containing ZSM-5 catalysts can produce C[sub 5][sup +] liquids from CH[sub 5] and O[sub 2] if dehydrogenation and oxidation functions of the metal are in balance. 12 refs., 4 tabs.},
doi = {10.1006/jcat.1994.1194},
journal = {Journal of Catalysis; (United States)},
number = ,
volume = 148:1,
place = {United States},
year = {Fri Jul 01 00:00:00 EDT 1994},
month = {Fri Jul 01 00:00:00 EDT 1994}
}