期刊
CHEMICAL ENGINEERING JOURNAL
卷 429, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.132278
关键词
Glycerol steam reforming; Ni-based catalyst; Metallurgical waste valorization; Kinetic modeling; Langmuir-Hinshelwood-Hougen-Watson reaction mechanism
资金
- Natural Sciences and Engineering Research Council of Canada (NSERC)
- Alexander Graham Bell Canada Graduate Scholarships Master's program (NSERC CGS M)
- Centre for Innovation and Research on Carbon Utilisation in Industrial Technologies (CIRCUIT)
The study investigated the kinetics of glycerol steam reforming reaction catalyzed by a nickel-promoted metallurgical residue in a fixed-bed reactor at atmospheric pressure. The most accurate and thermodynamically consistent mechanism involved the dissociative adsorption of glycerol, which led to the breaking of C-C bonds and dehydrogenation of glycerol as the rate-determining step. The activation energy was found to be 66.1 kJ.mol-1 with a partial order with respect to glycerol of 0.63, as validated by a macroscopic analysis of glycerol to gas consumption rates.
The kinetics of the glycerol steam reforming reaction catalyzed by a nickel-promoted metallurgical residue was studied in a fixed-bed reactor at atmospheric pressure. The temperature was varied between 480 degrees C and 580 degrees C. The experimental reaction rates were correlated via different heterogeneous kinetic models based on LangmuirHinshelwood-Hougen-Watson mechanisms that consider single- or dual-site adsorption of the reactants. The mechanism that provided the most mathematically accurate and thermodynamically consistent results is initiated by dissociative adsorption of glycerol, which cause the breaking of two C-C bonds in the glycerol molecule upon adsorption. This model claims that the dehydrogenation of an adsorbed glycerol intermediate is the ratedetermining step of the global reaction. A macroscopic analysis of the glycerol to gas consumption rates also validated the activation energies identified by the successful heterogeneous model by fitting the experimental data to a straightforward power law model. The activation energy was found to be 66.1 kJ.mol- 1 with a partial order with respect to glycerol of 0.63.
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