Analysis of light-off during oxidation of reactant mixtures on Pt/Al2O3 using micro-kinetic models

Kota, Arun S.; Dadi, Rama Krishna; Luss, Dan; Balakotaiah, Vemuri

doi:10.1016/j.ces.2017.02.050

Title: Analysis of light-off during oxidation of reactant mixtures on Pt/Al₂O₃ using micro-kinetic models

Journal Article · Thu Mar 16 00:00:00 EDT 2017 · Chemical Engineering Science

DOI:https://doi.org/10.1016/j.ces.2017.02.050· OSTI ID:1533624

Kota, Arun S. ^[1]; Dadi, Rama Krishna ^[1]; Luss, Dan ^[1];

^[1]

University of Houston, TX (United States)

An elementary step mechanism, which accounts for adsorption, desorption and surface reaction steps is proposed for co-oxidation of CO, propylene, hydrogen and ethane on Pt/Al₂O₃. Parameter estimation is used to determine the kinetic parameters for these steps, which depend on platinum loading and dispersion. A micro-kinetic model is proposed for water-gas shift reaction that captures the experimental trend observed during co-oxidation of CO/H₂. This mechanism is used to predict hysteresis features during oxidation and co-oxidation reactions. The oxidation of all the individual reactants exhibits regular hysteresis and the model predicts the experimentally observed inverse hysteresis during co-oxidation of CO and C₃H₆. The inverse hysteresis is caused by surface intermediates formed during C₃H₆ oxidation. These surface intermediates block the active sites, decreasing the light-off activity of CO during ramp down. The developed micro-kinetic model can also explain steam reforming of propylene and ethane on Pt/Al₂O₃. We also compare the predicted hysteresis during CO oxidation by global and micro-kinetic models. The predicted ignition temperature by both global and micro-kinetic models is almost same. However, the predicted extinction temperature by the global and micro-kinetic models is rather different. This behavior is due to different rate determining step during ramp down period.

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Research Organization:: Univ. of Houston, TX (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Science Foundation (NSF)

Grant/Contract Number:: EE0000205; CBET-1258688

OSTI ID:: 1533624

Alternate ID(s):: OSTI ID: 1413356

Journal Information:: Chemical Engineering Science, Vol. 166, Issue C; ISSN 0009-2509

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 17 works

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Title: Analysis of light-off during oxidation of reactant mixtures on Pt/Al2O3 using micro-kinetic models

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Title: Analysis of light-off during oxidation of reactant mixtures on Pt/Al₂O₃ using micro-kinetic models