Details
| Original language | English |
|---|---|
| Pages (from-to) | 142-149 |
| Number of pages | 8 |
| Journal | Journal of Molecular Catalysis A: Chemical |
| Volume | 297 |
| Issue number | 2 |
| Early online date | 20 Sept 2008 |
| Publication status | Published - 14 Jan 2009 |
Abstract
In order to identify factors governing selectivity of an oxygen-conducting perovskite BaCoxFeyZrzO3-δ (BCFZ) membrane in the partial oxidation of methane and ethane, mechanistic aspects of product formation in these reactions were investigated with a millisecond time resolution using the temporal analysis of products (TAP) reactor. It was found that the selectivity depends on: (i) reduction degree of the perovskite surface; the higher the reduction degree, the higher the ethane and ethylene selectivity in methane and ethane oxidation, respectively, and (ii) contact time; short contact times favor partial selective oxidation. The influence of contact time on the ethylene selectivity in ethane oxidation at degrees of ethane conversion above 85% was experimentally proven in hollow fiber and disk membranes, which differ in the contact times. The low activity and selectivity in methane oxidation in the BCFZ perovskite membrane reactor were significantly increased, when the membrane on the hydrocarbon side was coated by a Ni-based steam reforming catalyst. This catalyst fulfils a double role: (i) it increases the oxygen transport through the perovskite membrane due to the high oxygen consumption, and (ii) it accelerates syngas production via deep methane oxidation followed by dry and steam reforming of methane. The syngas selectivity increases with an increase in the catalyst reduction degree, which is determined by the ratio of the rate of methane oxidation to the rate of oxygen permeation through the membrane.
Keywords
- Membrane reactor, Mixed conductor, ODE, Perovskite, POM, Syngas, TAP
ASJC Scopus subject areas
- Chemical Engineering(all)
- Catalysis
- Chemical Engineering(all)
- Process Chemistry and Technology
- Chemistry(all)
- Physical and Theoretical Chemistry
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In: Journal of Molecular Catalysis A: Chemical, Vol. 297, No. 2, 14.01.2009, p. 142-149.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Selective oxidation of CH4 and C2H6 over a mixed oxygen ion and electron conducting perovskite - A TAP and membrane reactors study
AU - Kondratenko, Evgenii V.
AU - Wang, Haihui
AU - Kondratenko, Vita A.
AU - Caro, Jürgen
PY - 2009/1/14
Y1 - 2009/1/14
N2 - In order to identify factors governing selectivity of an oxygen-conducting perovskite BaCoxFeyZrzO3-δ (BCFZ) membrane in the partial oxidation of methane and ethane, mechanistic aspects of product formation in these reactions were investigated with a millisecond time resolution using the temporal analysis of products (TAP) reactor. It was found that the selectivity depends on: (i) reduction degree of the perovskite surface; the higher the reduction degree, the higher the ethane and ethylene selectivity in methane and ethane oxidation, respectively, and (ii) contact time; short contact times favor partial selective oxidation. The influence of contact time on the ethylene selectivity in ethane oxidation at degrees of ethane conversion above 85% was experimentally proven in hollow fiber and disk membranes, which differ in the contact times. The low activity and selectivity in methane oxidation in the BCFZ perovskite membrane reactor were significantly increased, when the membrane on the hydrocarbon side was coated by a Ni-based steam reforming catalyst. This catalyst fulfils a double role: (i) it increases the oxygen transport through the perovskite membrane due to the high oxygen consumption, and (ii) it accelerates syngas production via deep methane oxidation followed by dry and steam reforming of methane. The syngas selectivity increases with an increase in the catalyst reduction degree, which is determined by the ratio of the rate of methane oxidation to the rate of oxygen permeation through the membrane.
AB - In order to identify factors governing selectivity of an oxygen-conducting perovskite BaCoxFeyZrzO3-δ (BCFZ) membrane in the partial oxidation of methane and ethane, mechanistic aspects of product formation in these reactions were investigated with a millisecond time resolution using the temporal analysis of products (TAP) reactor. It was found that the selectivity depends on: (i) reduction degree of the perovskite surface; the higher the reduction degree, the higher the ethane and ethylene selectivity in methane and ethane oxidation, respectively, and (ii) contact time; short contact times favor partial selective oxidation. The influence of contact time on the ethylene selectivity in ethane oxidation at degrees of ethane conversion above 85% was experimentally proven in hollow fiber and disk membranes, which differ in the contact times. The low activity and selectivity in methane oxidation in the BCFZ perovskite membrane reactor were significantly increased, when the membrane on the hydrocarbon side was coated by a Ni-based steam reforming catalyst. This catalyst fulfils a double role: (i) it increases the oxygen transport through the perovskite membrane due to the high oxygen consumption, and (ii) it accelerates syngas production via deep methane oxidation followed by dry and steam reforming of methane. The syngas selectivity increases with an increase in the catalyst reduction degree, which is determined by the ratio of the rate of methane oxidation to the rate of oxygen permeation through the membrane.
KW - Membrane reactor
KW - Mixed conductor
KW - ODE
KW - Perovskite
KW - POM
KW - Syngas
KW - TAP
UR - http://www.scopus.com/inward/record.url?scp=57749188958&partnerID=8YFLogxK
U2 - 10.1016/j.molcata.2008.09.015
DO - 10.1016/j.molcata.2008.09.015
M3 - Article
AN - SCOPUS:57749188958
VL - 297
SP - 142
EP - 149
JO - Journal of Molecular Catalysis A: Chemical
JF - Journal of Molecular Catalysis A: Chemical
SN - 1381-1169
IS - 2
ER -