Journal of Industrial and Engineering Chemistry, Vol.18, No.1, 266-271, January, 2012
A kinetic study of Pd-Au catalyzed synthesis of vinyl acetate from oxidation of ethylene and acetic acid in heterogeneous gas reaction
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While qualitative interpretation of the experimental results is often limited to the identification of global mechanistic phenomena, kinetic modeling is a more powerful tool for the identification of the chemical reaction network that can describe the experimental results. In this paper, kinetic study of vinyl acetate(VA) synthesis was performed in a fixed bed reactor with oxidation of ethylene and acetic acid in gaseous phase over Pd/Au/SiO2 catalyst under the industrial relevant reaction condition as follows: temperature of 120-165℃ , at constant pressure of 8 bar and the ratio of catalyst mass to the feed (W/F) was maintained at 70 g/mol min. Variation in partial pressure and concentration of reactants have led us to determine the rate limiting step and therefore proposing a new rate low based on Langmuir-Hinshelwood-Hougen-Watson (LHHW) approached consistent with experimental observation while adapted through mathematical formulation with high reliance. So, the kinetic parameters were determined by the Levenberg-Marquardt algorithm. Effect of temperature has also been surveyed showing a decreased in selectivity due to the difference in reaction constants of main and side reaction rate and an increase rate due to the increase in apparent activation energy.
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