This two-parts paper summarizes the experimental and theoretical results of a comprehensive and first of its kind study on the kinetics of carbon dioxide (CO2) absorption and desorption in and from aqueous solutions of monoethanolamine (MEA), diethanolamine (DEA), methyl-diethanolamine (MDEA) and 2-amino-2-methyl-1-propanol (AMP) and their mixtures (i.e., MEA + AMP, MEA + MDEA, DEA + AMP and DEA + MDEA). Part-1 of this paper presents a detailed design of the novel hemispherical apparatus and a rigorous mathematical model applicable to both absorption and desorption conditions with some preliminary results and Part-2 provides detailed results with estimates of kinetic coefficients for CO2 absorption and desorption for eight different aqueous amine systems. The new hemispherical contactor consists of a 76 mm diameter solid hemisphere housed in a Pyrex glass cylinder with appropriate gas and liquid feed and withdrawal systems. The liquid feed passes through a 4 mm ID tube, which is located in the center of the hemisphere, and discharges at the top. The liquid descends as a well-defined liquid film over the surface of the hemisphere and is collected by a funnel (79 mm ID) at the base of the hemisphere. The interfacial area and hydrodynamics are well defined and the entrance/exit effects as well as surface rippling are minimized. Using this apparatus, the absorption experiments were conducted at near atmospheric pressure with pure CO2 saturated with water vapor at 293-323 K with initially unloaded solutions and the desorption experiments were performed at 333-383 K for CO2 loadings between 0.02 and 0.7 moles Of CO2 per mole of amine using humidified nitrogen gas as a stripping medium at total system pressures up to 205 kPa. The new rigorous mathematical model developed to interpret the rate data is based on the principle of diffusional mass transfer accompanied with liquid-phase chemical reactions over a hemispherical liquid film. Also developed in this work is a methodology that uses the rigorous model in conjunction with a non-linear regression technique to estimate kinetic parameters. Preliminary results presented in this part of the paper show that the new experimental apparatus was successful in accurately measuring and the new model and its numerical implementation were successful in accurately predicting both absorption and desorption rates for all aqueous amine systems considered in this study. (c) 2006 Elsevier Ltd. All fights reserved.