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Boreskov Institute of Catalysis of the Siberian Branch of Russian ...

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OP-I-12honeycomb monolith matrices [3,4]. The simulation was fulfilled for all range <strong>of</strong> temperaturesand gas velocities given above. The analysis <strong>of</strong> inter-phase mass transfer influence on <strong>the</strong>reaction rate in this structured reactor was performed on <strong>the</strong> base <strong>of</strong> a one-dimensional modelwith evaluated mass transfer correlations and <strong>the</strong> restrictions on <strong>the</strong> catalyst activity forstudied operation conditions were defined, while <strong>the</strong> reaction occurs in <strong>the</strong> chemical orchemical-diffusion- controlled regime.POM reactionA number <strong>of</strong> experimental runs with variation <strong>of</strong> contact time, temperature and feedcomposition was fulfilled to study <strong>the</strong> dependence <strong>of</strong> <strong>the</strong> reagent (CH 4 and O 2 ) and product(H 2 , CO, CO 2 ) concentrations on <strong>the</strong> operation conditions. In all cases, <strong>the</strong> rise <strong>of</strong> temperatureand/or contact time leads to <strong>the</strong> increase <strong>of</strong> product selectivity. At high temperatures, whenoxygen is absent in <strong>the</strong> gas phase, such impact reveals <strong>the</strong> importance <strong>of</strong> indirect pathway <strong>of</strong>methane oxidation as well as <strong>the</strong> rise <strong>of</strong> CH 4 conversion and CO selectivity indicates <strong>the</strong>methane transformation through reforming reactions following <strong>the</strong> deep oxidation. At contacttime <strong>of</strong> 4.7 ms and temperatures below 750 °С, syngas is formed in <strong>the</strong> presence <strong>of</strong> oxygen. Itcould be supposed that <strong>the</strong> syngas generation can proceed by <strong>the</strong> direct selective oxidation <strong>of</strong>methane.The data were processed to estimate <strong>the</strong> rates and its kinetic parameters <strong>of</strong> <strong>the</strong> mainindependent reaction pathways on <strong>the</strong> catalyst developed. The experimental points for dataprocessing were selected with minimal influence <strong>of</strong> mass transfer according to <strong>the</strong> analysisgiven above as well as with minimal temperature gradients. The kinetic characteristics <strong>of</strong> deepmethane oxidation as well as steam and dry reforming were determined, and <strong>the</strong> contribution<strong>of</strong> <strong>the</strong> direct route <strong>of</strong> partial oxidation <strong>of</strong> methane was evaluated.Thus, <strong>the</strong> studies performed show that <strong>the</strong> suggested construction <strong>of</strong> <strong>the</strong> small scalereactor with separate structured element <strong>of</strong> a real catalyst is promising for <strong>the</strong> kinetic studiesunder severe conditions. This reactor can be used also as effective tool to predict <strong>the</strong>characteristics <strong>of</strong> catalyst behavior for real industrial conditions.References1. G. Groppi, W. Ibashi, E. Tronconi, P. Forzatti, CEJ, 82 (2001) 57-71.2. S. Pavlova, N. Sazonova, V. Sadykov, S. Pokrovskaya, V. Kuzmin, G. Alikina, A. Lukashevich,E. Gubanova, <strong>Catalysis</strong> Today, 105 (2005) 367-371.3. R.D. Hawthorn, AIChE Symp. Ser. 70 (137) (1974) 428-438.4. E. Tronconi, P. Forzatti, AIChE J. 38 (1992) 201-210.49

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