Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 282, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2020.119408
Keywords
COx co-methanation; Intrinsic kinetic model; Surface kinetics; NiAlOx catalyst; Isotope effect studies
Funding
- TUM Graduate School
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The study developed a kinetic model to describe the competitive adsorption mechanism of CO and CO2 in the methanation reaction, and the influence of the decomposition of the hydrogenated COHy intermediate on the reaction rate.
The kinetics of the gas-phase co-methanation reaction of carbon oxides over a co-precipitated 44 wt.% NiAlOx catalyst were modelled via competitive adsorption of CO and CO2 and the subsequent methanation of a common surface intermediate. Steady-state isotope experiments and model discrimination suggest the decomposition of a hydrogenated COHy surface intermediate to be the kinetically relevant step in the methanation reaction. The best fit is obtained for hydroxycarbene (y = 2). The presented kinetic model is the first to explicitly describe the full coupling of CO and CO2 transformation. It is built on the basis of CO methanation, CO2 methanation, steam reforming, and water-gas shift experiments over a wide range of conditions. All model parameters are thermodynamically consistent and statistically relevant.
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