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Intrinsic kinetics of low temperature catalytic methane–steam reforming and water–gas shift over Rh/CeαZr1−αO2 catalyst

Paper ID Volume ID Publish Year Pages File Format Full-Text
41883 45903 2010 12 PDF Available
Title
Intrinsic kinetics of low temperature catalytic methane–steam reforming and water–gas shift over Rh/CeαZr1−αO2 catalyst
Abstract

This paper presents the intrinsic kinetics of CH4 steam reforming developed over Rh/Ce0.6Zr0.4O2 catalyst in a relatively low temperature range of 475–575 °C and 1.5 bar pressure. The kinetic experiments are conducted in an integral fixed bed reactor with no mass and heat transport limitations and far from equilibrium conditions. Therefore, intrinsic reaction rate measurements are guaranteed. The model is based upon two-site adsorption surface hypothesis, and 14 elementary reaction steps are postulated. CH4 is dissociatively adsorbed onto the Rh active sites, and steam is dissociatively adsorbed on the ceria support active sites as an influential adsorption surface shown in the model. Therefore, no competition between CH4 and steam in adsorbing on the same site surface is observed. The kinetic rate expressions are derived according to the Langmuir–Hinshelwood formalism. The redox surface reactions between the carbon containing species and the lattice oxygen leading to CO and CO2 formation are considered as rate determining steps. The inhibitory effect of gaseous product species is also reflected in the kinetics. The model is found to be statistically accurate and thermodynamically consistent. The estimated activation energies and adsorption enthalpies are in agreement with literature for CH4 steam reforming reaction over Rh. The reaction kinetics is validated by steam reforming experiments at 550 °C and 1.5 bar using 150 mg catalyst in a diluted bed of 5 cm length. The kinetic model is implemented in a one-dimensional pseudo-homogenous plug flow reactor model and thus simulated at identical experimental conditions. The simulation results are in excellent agreement with the experimental values.

Graphical abstractFigure optionsDownload full-size imageDownload high-quality image (105 K)Download as PowerPoint slideResearch highlights▶ The intrinsic kinetics of CH4 steam reforming is developed over Rh/Ce0.6Zr0.4O2. ▶ The model is based upon two-site adsorption surface hypothesis in a low temperature. ▶ The redox surface reactions are considered as rate determining steps. ▶ The inhibitory effect of gaseous product species is reflected in the kinetics. ▶ Rh-based steam reforming kinetics is compared to Ni-based catalyst kinetics.

Keywords
Methane steam reforming; Intrinsic reaction kinetics; Water–gas shift; Reaction mechanism; Rhodium-based catalyst; Ceria–zirconia supported catalyst
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Intrinsic kinetics of low temperature catalytic methane–steam reforming and water–gas shift over Rh/CeαZr1−αO2 catalyst
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Publisher
Database: Elsevier - ScienceDirect
Journal: Applied Catalysis A: General - Volume 389, Issues 1–2, 1 December 2010, Pages 80–91
Authors
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Subjects
Physical Sciences and Engineering Chemical Engineering Catalysis
Get Full-Text Now
Don't Miss Today's Special Offer
Price was $35.95
You save - $31
Price after discount Only $4.95
100% Money Back Guarantee
Full-text PDF Download
Online Support
Any Questions? feel free to contact us