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Title: Selective methane oxidation over promoted oxide catalysts. Quarterly technical progress report, June 1, 1993--August 31, 1993

Abstract

At 550{degree}C, the 1 wt % SO{sub 4}{sup 2}{minus}/l wt % Sr/La{sub 2}O{sub 3} catalyst, one of the most active catalyst for the selective conversion of methane at these moderate temperatures, showed a very good stability with a reactant mixture of CH{sub 4}/air = 1/1 with GHSV = 70,040 {ell}/kg catal/hr. During a 25 hr catalytic test, the conversion of CH{sub 4} and the C{sub 2}{sup +} selectivity did not change, indicating good stability of the catalyst. At the same time, the CO{sub 2}/CO ratio remained steady at about 2.2, but the C{sup 2}{sup =}/C{sub 2} ratio shifted slightly with time from 0.74 to 0.68. The oxidative coupling of CH{sub 4} to C{sub 2}-hydrocarbons was very sensitive at 550{degree}C to the alteration of the CH{sub 4}/air reactant ratio at GHSV = 70,040 {ell}/kg catal/hr. It was observed that the conversion of CH{sub 4}, the C{sub 2}{sup +} selectivity, and the %yield of C{sub 2}{sup +} hydrocarbon products decreased very rapidly with increasing CH{sub 4}/air ratio from 1 to 3-4. At the largest CH{sub 4}/air ratio of 40.77 that was used utilized, the CH{sub 4} conversion was less than 0-5 C-mol%. The reverse process of decreasing the CH{sub 4}/air ratio frommore » {approx}40 to 1 showed nearly reversible catalytic performance, but some deactivation was apparent at the lowest reactant ratios. The 1 wt % SO{sub 4}{sup 2}{minus}/1 wt % Sr/La{sub 2}O{sub 3} catalyst used in the experiments in which the CH{sub 4}/air ratio was varied subsequently revealed a good stability in the CH{sub 4} conversion level during testing at 550{degree}C for 15 hr (GHSV = 70,040 {ell}/kg catal/hr and CH{sub 4}/air = 1/1). Indeed, the C{sub 2}{sup +} selectivity even increased by 3 to 4 C-mol%. Increasing the temperature from 550 to 600{degree}C resulted in a further recovery of the activity of the partially deactivated catalyst.« less

Authors:
; ; ;
Publication Date:
Research Org.:
Lehigh Univ., Bethlehem, PA (United States)
Sponsoring Org.:
USDOE, Washington, DC (United States)
OSTI Identifier:
10118771
Report Number(s):
DOE/MC/29228-3579
ON: DE94005909; BR: AB0530150/AC0535000
DOE Contract Number:  
FG21-92MC29228
Resource Type:
Technical Report
Resource Relation:
Other Information: PBD: Sep 1993
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 01 COAL, LIGNITE, AND PEAT; METHANE; OXIDATION; CATALYSTS; LANTHANUM OXIDES; CATALYTIC EFFECTS; SPECIFICITY; PROGRESS REPORT; 400201; 010408; CHEMICAL AND PHYSICOCHEMICAL PROPERTIES; C1 PROCESSES

Citation Formats

Klier, K, Herman, R G, Sarkany, J, and Sun, Qun. Selective methane oxidation over promoted oxide catalysts. Quarterly technical progress report, June 1, 1993--August 31, 1993. United States: N. p., 1993. Web. doi:10.2172/10118771.
Klier, K, Herman, R G, Sarkany, J, & Sun, Qun. Selective methane oxidation over promoted oxide catalysts. Quarterly technical progress report, June 1, 1993--August 31, 1993. United States. doi:10.2172/10118771.
Klier, K, Herman, R G, Sarkany, J, and Sun, Qun. Wed . "Selective methane oxidation over promoted oxide catalysts. Quarterly technical progress report, June 1, 1993--August 31, 1993". United States. doi:10.2172/10118771. https://www.osti.gov/servlets/purl/10118771.
@article{osti_10118771,
title = {Selective methane oxidation over promoted oxide catalysts. Quarterly technical progress report, June 1, 1993--August 31, 1993},
author = {Klier, K and Herman, R G and Sarkany, J and Sun, Qun},
abstractNote = {At 550{degree}C, the 1 wt % SO{sub 4}{sup 2}{minus}/l wt % Sr/La{sub 2}O{sub 3} catalyst, one of the most active catalyst for the selective conversion of methane at these moderate temperatures, showed a very good stability with a reactant mixture of CH{sub 4}/air = 1/1 with GHSV = 70,040 {ell}/kg catal/hr. During a 25 hr catalytic test, the conversion of CH{sub 4} and the C{sub 2}{sup +} selectivity did not change, indicating good stability of the catalyst. At the same time, the CO{sub 2}/CO ratio remained steady at about 2.2, but the C{sup 2}{sup =}/C{sub 2} ratio shifted slightly with time from 0.74 to 0.68. The oxidative coupling of CH{sub 4} to C{sub 2}-hydrocarbons was very sensitive at 550{degree}C to the alteration of the CH{sub 4}/air reactant ratio at GHSV = 70,040 {ell}/kg catal/hr. It was observed that the conversion of CH{sub 4}, the C{sub 2}{sup +} selectivity, and the %yield of C{sub 2}{sup +} hydrocarbon products decreased very rapidly with increasing CH{sub 4}/air ratio from 1 to 3-4. At the largest CH{sub 4}/air ratio of 40.77 that was used utilized, the CH{sub 4} conversion was less than 0-5 C-mol%. The reverse process of decreasing the CH{sub 4}/air ratio from {approx}40 to 1 showed nearly reversible catalytic performance, but some deactivation was apparent at the lowest reactant ratios. The 1 wt % SO{sub 4}{sup 2}{minus}/1 wt % Sr/La{sub 2}O{sub 3} catalyst used in the experiments in which the CH{sub 4}/air ratio was varied subsequently revealed a good stability in the CH{sub 4} conversion level during testing at 550{degree}C for 15 hr (GHSV = 70,040 {ell}/kg catal/hr and CH{sub 4}/air = 1/1). Indeed, the C{sub 2}{sup +} selectivity even increased by 3 to 4 C-mol%. Increasing the temperature from 550 to 600{degree}C resulted in a further recovery of the activity of the partially deactivated catalyst.},
doi = {10.2172/10118771},
journal = {},
number = ,
volume = ,
place = {United States},
year = {1993},
month = {9}
}