Journal
CHEMICAL ENGINEERING SCIENCE
Volume 66, Issue 24, Pages 6441-6452Publisher
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ces.2011.08.055
Keywords
Heterogeneous catalysis; Transient kinetics; Temporal Analysis of Products (TAP); Thin-zone; Y-Procedure; Irreversible adsorption
Categories
Funding
- CREL consortium at Washington University in Saint Louis
- Ghent University [BOF/GOA 01GA0405]
- Flemish Government
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This paper deals with the analysis of transient kinetic data obtained in the Thin-Zone (TZ) configuration of the Temporal Analysis of Products (TAP) reactor. The Y-procedure that reconstructs the reaction rate and gas composition in the catalytic zone with no assumptions on the reaction mechanism (Yablonsky et al., 2007) was applied to irreversible adsorption with coverage-dependent kinetic coefficients. We have used the Y-Procedure analysis to develop a novel framework for the interpretation of non-steady-state kinetic data. This framework was illustrated by multiple numerical examples concerning irreversible adsorption, and by experimental data corresponding to oxygen adsorption on polycrystalline platinum. The total concentration of active sites was estimated as 6 x 10(-7) mol/g(cat). It was found that for the surface coverage up to 0.8, kinetics followed the dissociative adsorption model with an intrinsic adsorption constant of 1.12 x 10(6) m(3)/mol/s. Kinetic parameters estimated via the Y-procedure agreed well with the values obtained via the moment analysis. The methodology developed in this paper will guide the systematic application of the Y-Procedure analysis to more complex catalytic systems. (C) 2011 Elsevier Ltd. All rights reserved.
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