Kinetic Modeling of the SWNT Growth by CO Disproportionation on CoMo Catalysts
A kinetic model has been developed to describe the growth of single-walled carbon nanotubes (SWNT) in the CoMoCAT™ method, which is based on the disproportionation of CO on supported CoMo catalysts. The model attempts to capture mathematically the different stages involved in this method: (i) catalyst activation or in-situ creation of active sites, i.e., reduced Co clusters by transformation of CoMoOx precursor species, or oxidized sites; (ii) CO decomposition over active sites, which increases the surface fugacity of carbon until reaching a certain threshold; (iii) nucleation of ordered forms of carbon; (iv) C diffusion (both across the surface and into the metal particle); (v) SWNT growth; (vi) termination, by either deactivation of the catalyst active sites or by increase in the carbon concentration at the metal/SWNT interface, approaching that of the metal/gas interface and eliminating the driving force for diffusion. Previous investigations have only explained the growth termination by the former. Here, we emphasize the possible contribution of the later and propose a novel "hindrance factor" to quantify the effect of nanotube interaction with its surroundings on the growth termination. To test the kinetic model and obtain typical values of the physical parameters, experiments have been conducted on a CoMo/SiO2 catalyst in a laboratory flow reactor, in which the rate of carbon deposition was continuously evaluated by the direct measurement of the CO2 evolution as a function of time. The experimental data are fitted very well with model.
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Document Type: Research Article
Publication date: 01 November 2008
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