NDLI: Methane Steam Reforming Kinetics on a Ni/Mg/K/Al$_{2}$O$

Content Provider	Springer Nature Link
Author	Robinson, Allison M. Gin, Megan E. Yung, Matthew M.
Copyright Year	2013
Abstract	The kinetics of methane steam reforming were studied on a Ni/Mg/K/Al$_{2}$O$_{3}$ catalyst that was developed for conditioning of biomass-derived syngas. Reactions were conducted in a packed-bed reactor while the concentrations of reactants (methane and steam) and products (hydrogen, carbon monoxide, and carbon dioxide) were varied at atmospheric pressure, with the effects of temperature (525–700 °C) and residence time also being investigated. A power law rate model was developed using nonlinear regression to provide a predictive capability for the rate of methane conversion over this catalyst, to be used for reactor design and technoeconomic analysis of process designs. In order to provide some mechanistic insight, and to compare this catalyst to other non-promoted Ni/Al$_{2}$O$_{3}$ catalysts reported in the literature, a reaction mechanism consisting of five elementary steps, using a Langmuir–Hinshelwood type approach, was also considered. These five steps included: (i) CH$_{4}$ adsorption, (ii) H$_{2}$O adsorption, (iii) surface reaction of adsorbed CH$_{4}$ and H$_{2}$O to form CO and H$_{2}$, (iv) CO desorption, and (v) H$_{2}$ desorption. Nonlinear regression was then used to fit each of the rate laws to the experimental data. From these results, the model that assumed CH$_{4}$ adsorption to be the rate determining step provided the best fit of the experimental data. This finding is consistent with literature studies on non-promoted Ni/Al$_{2}$O$_{3}$ catalysts, in which methane adsorption has been proposed to be the rate determining step during catalytic methane steam reforming. Both the power rate laws and the rate law assuming CH$_{4}$ adsorption to be the rate determining step can be used as predictive tools for determining methane conversion for a given set of process conditions. Additionally, a rate expression that assumed the rate was only a function of methane partial pressure was considered, namely, $$rate = kP_{{CH_{4} }}$$ , where $$k = k_{0} e^{{^{{ - {\text{Ea}}/{\text{RT}}}} }}$$ , with P$_{CH4}$ in units of Torr. This first-order-methane rate expression fit the data well, yielding an apparent activation energy over this catalyst of E$_{a}$ = 93 kJ/mol and the pre-exponential rate constant of k$_{0}$ = 7.67 × 10$^{5}$ mol/(g-cat s Torr CH$_{4}$).
Starting Page	1708
Ending Page	1715
Page Count	8
File Format	PDF
ISSN	10225528
Journal	Topics in Catalysis
Volume Number	56
Issue Number	18-20
e-ISSN	15729028
Language	English
Publisher	Springer US
Publisher Date	2013-07-11
Publisher Place	New York
Access Restriction	One Nation One Subscription (ONOS)
Subject Keyword	Methane steam reforming Rate law Nickel catalyst Biomass conditioning Kinetics Catalysis Physical Chemistry Pharmacy Industrial Chemistry/Chemical Engineering Characterization and Evaluation of Materials
Content Type	Text
Resource Type	Article
Subject	Chemistry Catalysis

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