Kinetics of carbon dioxide absorption and desorption in aqueous alkanolamine solutions using a novel hemispherical contactor—II: Experimental results and parameter estimation

Abstract

In Part 1 of this paper, detailed design of the hemispherical apparatus and a rigorous mathematical model applied to CO2 absorption and desorption in and from aqueous alkanolamine solutions was presented with some preliminary results. This part of the paper provides detailed results on CO2–amine kinetics under absorption and desorption conditions and present new estimates of the kinetic parameter for aqueous solutions of monoethanolamine (MEA), diethanolamine (DEA), methyl-diethanolamine (MDEA) and 2-amino-2-methyl-1-propanol (AMP). The absorption experiments were conducted at near atmospheric pressure with pure humidified CO2 at 293–323 K using initially unloaded solutions. The desorption experiments were performed at 333–383 K for CO2 loadings between 0.02 to 0.7 mol of CO2 per mole of amine using humidified nitrogen gas as a stripping medium at total system pressure ranging from 110 to 205 kPa.

The new rigorous mathematical model discussed in Part 1 was used in conjunction with a non-linear regression technique to estimate the kinetic parameters. In all cases, the new model predicts the experimental results well. Also, the new results clearly demonstrate that the theory of absorption with reversible chemical reaction could be used to predict desorption rates. The zwitterion mechanism adequately describes the reactions between CO2 and carbamate forming amines such as MEA, DEA and AMP. The reactions between CO2 and aqueous MDEA solutions are best described by a base-catalyzed hydration reaction mechanism. The kinetic data obtained show that desorption experiments could be used to determine both forward and backward rate constants accurately. The absorption experiments, on the other hand, could only be used to determine forward rate constants. It was found that at all operating conditions used in this study, the kinetic parameters for MEA, DEA and AMP obtained using absorption data could not be extrapolated to predict desorption rates. However, for MDEA, these data could be used successfully to obtain reasonably good predictions of desorption rates.