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

Abstract

A 1 wt% SO{sub 4}{sup 2{minus}}/1 wt% Sr/La{sub 2}O{sub 3} catalyst has been shown by us to be one of the most active catalyst for the oxidative coupling of CH{sub 4} to C{sub 2} hydrocarbons. One of the by-products is CO{sub 2} and this is a potential strong poison for the formation of C{sub 2}{sup +} products. Hence, various pretreatments of this catalyst were studied in terms of effect on the catalytic performance. Before the reaction was carried out at 500 or 550{degrees}C, the catalyst was pretreated in flowing air or He at 500, 700, or 800{degrees}C. Relative to the 500{degrees}C treatment, the pretreatment in air at 700{degrees}C only slightly decreased the C{sub 2}{sup +} selectivity while the CO{sub x} selectivity increased. This effect was larger when the pretreatment was carried out at 800{degrees}C. It was observed that the deactivation effect was slightly smaller when the pretreatments were carried out in He instead of air. For both air and He, the CH{sub 4}, conversion and the C{sub 2} %yield showed more or less parallel changes (small decreases) with increasing pretreatment temperature. After a standard pretreatment (air, 500{degrees}C, 1 hr), the reaction temperature was increased stepwise from 500 to 700{degrees}C andmore » then lowered to 550 (or 500){degrees}C. It was observed that the catalytic performance showed deactivation towards the C{sub 2}{sup +} products. Decreasing stepwise the total flow rate (GHSV) of the reacting gas mixture (CH{sub 4}/air = 1/1) from 70,175 to 5,388 {ell}/kg catal/hr at a reaction temperature of 550{degrees}C caused large changes in both the activity and selectivity. After going back at 550{degrees}C to the original GHSV = 70,175 {ell}/kg catal/hr, the temperature was increased stepwise up to 600{degrees}C. Up to 580{degrees}C, the catalytic activity and selectivity did not change very much.« less

Authors:
; ; ;
Publication Date:
Research Org.:
Lehigh Univ., Bethlehem, PA (United States). Zettlemoyer Center for Surface Studies
Sponsoring Org.:
USDOE, Washington, DC (United States)
OSTI Identifier:
10176534
Report Number(s):
DOE/MC/29228-3408
ON: DE93040001
DOE Contract Number:  
FG21-92MC29228
Resource Type:
Technical Report
Resource Relation:
Other Information: PBD: Jun 1993
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 10 SYNTHETIC FUELS; 01 COAL, LIGNITE, AND PEAT; OXIDATION; CATALYSTS; METHANE; SULFATES; CATALYTIC EFFECTS; STRONTIUM; LANTHANUM OXIDES; PROGRESS REPORT; TEMPERATURE DEPENDENCE; METHANOL; FORMALDEHYDE; OXYGEN; AIR; SPECIFICITY; 400201; 100200; 010408; CHEMICAL AND PHYSICOCHEMICAL PROPERTIES; PRODUCTION; C1 PROCESSES

Citation Formats

Klier, K, Herman, R G, Sarkany, J, and Sun, Q. Selective methane oxidation over promoted oxide catalysts. Quarterly technical progress report, March 1, 1993--May 31, 1993. United States: N. p., 1993. Web. doi:10.2172/10176534.
Klier, K, Herman, R G, Sarkany, J, & Sun, Q. Selective methane oxidation over promoted oxide catalysts. Quarterly technical progress report, March 1, 1993--May 31, 1993. United States. doi:10.2172/10176534.
Klier, K, Herman, R G, Sarkany, J, and Sun, Q. Tue . "Selective methane oxidation over promoted oxide catalysts. Quarterly technical progress report, March 1, 1993--May 31, 1993". United States. doi:10.2172/10176534. https://www.osti.gov/servlets/purl/10176534.
@article{osti_10176534,
title = {Selective methane oxidation over promoted oxide catalysts. Quarterly technical progress report, March 1, 1993--May 31, 1993},
author = {Klier, K and Herman, R G and Sarkany, J and Sun, Q},
abstractNote = {A 1 wt% SO{sub 4}{sup 2{minus}}/1 wt% Sr/La{sub 2}O{sub 3} catalyst has been shown by us to be one of the most active catalyst for the oxidative coupling of CH{sub 4} to C{sub 2} hydrocarbons. One of the by-products is CO{sub 2} and this is a potential strong poison for the formation of C{sub 2}{sup +} products. Hence, various pretreatments of this catalyst were studied in terms of effect on the catalytic performance. Before the reaction was carried out at 500 or 550{degrees}C, the catalyst was pretreated in flowing air or He at 500, 700, or 800{degrees}C. Relative to the 500{degrees}C treatment, the pretreatment in air at 700{degrees}C only slightly decreased the C{sub 2}{sup +} selectivity while the CO{sub x} selectivity increased. This effect was larger when the pretreatment was carried out at 800{degrees}C. It was observed that the deactivation effect was slightly smaller when the pretreatments were carried out in He instead of air. For both air and He, the CH{sub 4}, conversion and the C{sub 2} %yield showed more or less parallel changes (small decreases) with increasing pretreatment temperature. After a standard pretreatment (air, 500{degrees}C, 1 hr), the reaction temperature was increased stepwise from 500 to 700{degrees}C and then lowered to 550 (or 500){degrees}C. It was observed that the catalytic performance showed deactivation towards the C{sub 2}{sup +} products. Decreasing stepwise the total flow rate (GHSV) of the reacting gas mixture (CH{sub 4}/air = 1/1) from 70,175 to 5,388 {ell}/kg catal/hr at a reaction temperature of 550{degrees}C caused large changes in both the activity and selectivity. After going back at 550{degrees}C to the original GHSV = 70,175 {ell}/kg catal/hr, the temperature was increased stepwise up to 600{degrees}C. Up to 580{degrees}C, the catalytic activity and selectivity did not change very much.},
doi = {10.2172/10176534},
journal = {},
number = ,
volume = ,
place = {United States},
year = {1993},
month = {6}
}