Kinetic and selectivity studies of gas-liquid reaction under Taylor flow in a circular capillary

The catalytic hydrogenation of 2-butyne- 1,4-diol to cis-2-butene- 1,4-diol and butane- 1,4-diol was carried out in a circular capillary operating in co-current down-flow mode in order to n-timic the behaviour of a monolith channel. The selected model reaction was performed over a 4 wt.% palladium/alumina catalyst using 30% (v/v) isopropanol/water solvent. Liquid and gas superficial velocities were varied over a wide range (0.0098 <V-SG <0.0356 m s(-1) and 0.0074 <V-SL <0. 1485 m s(-1)) in order to study the effect of gas bubble and liquid slug lengths on the observed reaction rate and selectivity towards cis-2-butene- 1,4-diol. At constant V-SG, upon increasing V-SL the reaction rate was sensitive to liquid slug length (Ls) and flow pattern such that the maximum reaction rate occurred at L-S/D = 1.2. While at constant VSL, upon increasing V-SG the reaction rate was influenced by both gas (L-G) and liquid slug lengths, decreasing from 0.0012 mol l(-1) min(-1) to reach a steady value. Varying the liquid slug length caused the selectivity to increase from 20 to 88%, whilst varying the gas slug length had a smaller effect, whereupon the selectivity slightly decreased from 95 to 83.6%. A model was developed to predict the concentration profiles of reactants and products incorporating a Langmuir-Hinshelwood model of the kinetics and correlations for estimating mass transfer coefficients from the literature. (C) 2007 Elsevier B.V. All rights reserved.