Analysis of heterogeneous oxygen exchange and fuel oxidation on the catalytic surface of perovskite membranes
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 activ...
| Main Authors: | , , |
|---|---|
| Other Authors: | |
| Format: | Article |
| Language: | en_US |
| Published: |
Elsevier
2016
|
| Online Access: | http://hdl.handle.net/1721.1/105396 https://orcid.org/0000-0001-8730-272X |
| _version_ | 1826211613105979392 |
|---|---|
| author | Kirchen, Patrick Hong, Jongsup Ghoniem, Ahmed F |
| author2 | Massachusetts Institute of Technology. Department of Mechanical Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Mechanical Engineering Kirchen, Patrick Hong, Jongsup Ghoniem, Ahmed F |
| author_sort | Kirchen, Patrick |
| collection | MIT |
| description | 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. |
| first_indexed | 2024-09-23T15:08:45Z |
| format | Article |
| id | mit-1721.1/105396 |
| institution | Massachusetts Institute of Technology |
| language | en_US |
| last_indexed | 2024-09-23T15:08:45Z |
| publishDate | 2016 |
| publisher | Elsevier |
| record_format | dspace |
| spelling | mit-1721.1/1053962024-06-26T20:38:16Z Analysis of heterogeneous oxygen exchange and fuel oxidation on the catalytic surface of perovskite membranes Kirchen, Patrick Hong, Jongsup Ghoniem, Ahmed F Massachusetts Institute of Technology. Department of Mechanical Engineering Hong, Jongsup Ghoniem, Ahmed F 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. King Abdullah University of Science and Technology (KAUST) (grant number KSU-I1-010-01) King Fahd University of Petroleum and Minerals (Center for Clean Water and Clean Energy at MIT and KFUPM) 2016-11-22T15:02:44Z 2016-11-22T15:02:44Z 2013-06 2013-05 Article http://purl.org/eprint/type/JournalArticle 03767388 http://hdl.handle.net/1721.1/105396 Hong, Jongsup, Patrick Kirchen, and Ahmed F. Ghoniem. “Analysis of Heterogeneous Oxygen Exchange and Fuel Oxidation on the Catalytic Surface of Perovskite Membranes.” Journal of Membrane Science 445 (October 2013): 96-106. https://orcid.org/0000-0001-8730-272X en_US http://dx.doi.org/10.1016/j.memsci.2013.05.055 Journal of Membrane Science Creative Commons Attribution-NonCommercial-NoDerivs License http://creativecommons.org/licenses/by-nc-nd/4.0/ application/pdf Elsevier Prof. Ghoniem via Angie Locknar |
| spellingShingle | Kirchen, Patrick Hong, Jongsup Ghoniem, Ahmed F Analysis of heterogeneous oxygen exchange and fuel oxidation on the catalytic surface of perovskite membranes |
| title | Analysis of heterogeneous oxygen exchange and fuel oxidation on the catalytic surface of perovskite membranes |
| title_full | Analysis of heterogeneous oxygen exchange and fuel oxidation on the catalytic surface of perovskite membranes |
| title_fullStr | Analysis of heterogeneous oxygen exchange and fuel oxidation on the catalytic surface of perovskite membranes |
| title_full_unstemmed | Analysis of heterogeneous oxygen exchange and fuel oxidation on the catalytic surface of perovskite membranes |
| title_short | Analysis of heterogeneous oxygen exchange and fuel oxidation on the catalytic surface of perovskite membranes |
| title_sort | analysis of heterogeneous oxygen exchange and fuel oxidation on the catalytic surface of perovskite membranes |
| url | http://hdl.handle.net/1721.1/105396 https://orcid.org/0000-0001-8730-272X |
| work_keys_str_mv | AT kirchenpatrick analysisofheterogeneousoxygenexchangeandfueloxidationonthecatalyticsurfaceofperovskitemembranes AT hongjongsup analysisofheterogeneousoxygenexchangeandfueloxidationonthecatalyticsurfaceofperovskitemembranes AT ghoniemahmedf analysisofheterogeneousoxygenexchangeandfueloxidationonthecatalyticsurfaceofperovskitemembranes |