Analysis of heterogeneous oxygen exchange and fuel oxidation on the catalytic surface of perovskite membranes

Handle URI:
http://hdl.handle.net/10754/597558
Title:
Analysis of heterogeneous oxygen exchange and fuel oxidation on the catalytic surface of perovskite membranes
Authors:
Hong, Jongsup; Kirchen, Patrick; Ghoniem, Ahmed F.
Abstract:
The catalytic kinetics of oxygen surface exchange and fuel oxidation for a perovskite membrane is investigated in terms of the thermodynamic state in the immediate vicinity of or on the membrane surface. Perovskite membranes have been shown to exhibit both oxygen perm-selectivity and catalytic activity for hydrocarbon conversion. A fundamental description of their catalytic surface reactions is needed. In this study, we infer the kinetic parameters for heterogeneous oxygen surface exchange and catalytic fuel conversion reactions, based on permeation rate measurements and a spatially resolved physical model that incorporates detailed chemical kinetics and transport in the gas-phase. The conservation equations for surface and bulk species are coupled with those of the gas-phase species through the species production rates from surface reactions. It is shown that oxygen surface exchange is limited by dissociative/associative adsorption/desorption of oxygen molecules onto/from the membrane surface. On the sweep side, while the catalytic conversion of methane to methyl radical governs the overall surface reactions at high temperature, carbon monoxide oxidation on the membrane surface is dominant at low temperature. Given the sweep side conditions considered in ITM reactor experiments, gas-phase reactions also play an important role, indicating the significance of investigating both homogeneous and heterogeneous chemistry and their coupling when examining the results. We show that the local thermodynamic state at the membrane surface should be considered when constructing and examining models of oxygen permeation and heterogeneous chemistry. © 2013 Elsevier B.V.
Citation:
Hong J, Kirchen P, Ghoniem AF (2013) Analysis of heterogeneous oxygen exchange and fuel oxidation on the catalytic surface of perovskite membranes. Journal of Membrane Science 445: 96–106. Available: http://dx.doi.org/10.1016/j.memsci.2013.05.055.
Publisher:
Elsevier BV
Journal:
Journal of Membrane Science
KAUST Grant Number:
KSU-I1-010-01
Issue Date:
Oct-2013
DOI:
10.1016/j.memsci.2013.05.055
Type:
Article
ISSN:
0376-7388
Sponsors:
The authors would like to thank the King Fahd University of Petroleum and Minerals (KFUPM) in Dhahran, Saudi Arabia, for funding the research reported in this paper through the Center of Clean Water and Clean Energy at Massachusetts Institute of Technology and KFUPM. This work is also supported by King Abdullah University of Science and Technology grant number KSU-I1-010-01.
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Full metadata record

DC FieldValue Language
dc.contributor.authorHong, Jongsupen
dc.contributor.authorKirchen, Patricken
dc.contributor.authorGhoniem, Ahmed F.en
dc.date.accessioned2016-02-25T12:42:01Zen
dc.date.available2016-02-25T12:42:01Zen
dc.date.issued2013-10en
dc.identifier.citationHong J, Kirchen P, Ghoniem AF (2013) Analysis of heterogeneous oxygen exchange and fuel oxidation on the catalytic surface of perovskite membranes. Journal of Membrane Science 445: 96–106. Available: http://dx.doi.org/10.1016/j.memsci.2013.05.055.en
dc.identifier.issn0376-7388en
dc.identifier.doi10.1016/j.memsci.2013.05.055en
dc.identifier.urihttp://hdl.handle.net/10754/597558en
dc.description.abstractThe catalytic kinetics of oxygen surface exchange and fuel oxidation for a perovskite membrane is investigated in terms of the thermodynamic state in the immediate vicinity of or on the membrane surface. Perovskite membranes have been shown to exhibit both oxygen perm-selectivity and catalytic activity for hydrocarbon conversion. A fundamental description of their catalytic surface reactions is needed. In this study, we infer the kinetic parameters for heterogeneous oxygen surface exchange and catalytic fuel conversion reactions, based on permeation rate measurements and a spatially resolved physical model that incorporates detailed chemical kinetics and transport in the gas-phase. The conservation equations for surface and bulk species are coupled with those of the gas-phase species through the species production rates from surface reactions. It is shown that oxygen surface exchange is limited by dissociative/associative adsorption/desorption of oxygen molecules onto/from the membrane surface. On the sweep side, while the catalytic conversion of methane to methyl radical governs the overall surface reactions at high temperature, carbon monoxide oxidation on the membrane surface is dominant at low temperature. Given the sweep side conditions considered in ITM reactor experiments, gas-phase reactions also play an important role, indicating the significance of investigating both homogeneous and heterogeneous chemistry and their coupling when examining the results. We show that the local thermodynamic state at the membrane surface should be considered when constructing and examining models of oxygen permeation and heterogeneous chemistry. © 2013 Elsevier B.V.en
dc.description.sponsorshipThe authors would like to thank the King Fahd University of Petroleum and Minerals (KFUPM) in Dhahran, Saudi Arabia, for funding the research reported in this paper through the Center of Clean Water and Clean Energy at Massachusetts Institute of Technology and KFUPM. This work is also supported by King Abdullah University of Science and Technology grant number KSU-I1-010-01.en
dc.publisherElsevier BVen
dc.subjectCatalytic fuel conversionen
dc.subjectCatalytic kineticsen
dc.subjectCatalytic membrane reactoren
dc.subjectOxygen surface exchangeen
dc.subjectPerovskite membraneen
dc.subjectSurface reactionen
dc.titleAnalysis of heterogeneous oxygen exchange and fuel oxidation on the catalytic surface of perovskite membranesen
dc.typeArticleen
dc.identifier.journalJournal of Membrane Scienceen
dc.contributor.institutionMassachusetts Institute of Technology, Cambridge, United Statesen
dc.contributor.institutionThe University of British Columbia, Vancouver, Canadaen
kaust.grant.numberKSU-I1-010-01en
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