Direct synthesis of acetic acid from CH4 andC02 by a step-wise route over Pd/SiO2 and Rh/SiO2 catalysts

The theoretical and experimental feasibility of direct conversion of CH4 and CO2 to acetic acid by an isothermal step-wise route over Pd/SiO2 and Rh/SiO2 catalysts was investigated. The methyl radical formation from CH4 dissociation and CO2 inserting into the intermediate are regarded as two limiting steps. Preliminary experimental results have shown that the following step-wise route can circumvent the thermodynamic limitation of this direct synthesis at low temperatures. Pd catalysts are more active than Rh catalysts at 170 degrees C and 200 degrees C, while formic acid is only produced on Pd catalysts. The optimum contact time of CH4 and CO2 with catalysts is 1 min under the experimental conditions. And there is no apparent deactivation resulting from carbon deposition for catalysts during the successive reaction cycles. (C) 2006 Elsevier B.V. All rights reserved.