Analysis of heterogeneous oxygen exchange and fuel oxidation on the catalytic surface of perovskite membranes
Name
J.Hong et al. Journal of Membrane Science 445 2013 96-106.pdf
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1.44 MB
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Checksum (MD5)
2ea51ef128bdf5c4bda1d6237028e57f
Author(s)
Kirchen, Patrick
Hong, Jongsup
Ghoniem, Ahmed F
Date Issued
June 2013
Journal
Journal of Membrane Science
Publisher
Elsevier
Citation
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.
Version
Author's final manuscript
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.
MIT Department
Massachusetts Institute of Technology. Department of Mechanical Engineering
Terms of Use
Creative Commons Attribution-NonCommercial-NoDerivs License
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DOI of Published Version
https://doi.org/10.1016/j.memsci.2013.05.055
