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Etude thermodynamique de la dissolution du dioxyde de carbone dans des solutions aqueuses d'alcanolamines

Hugues Arcis 1
1 TIM
Department of Chemistry, ICCF - Institut de Chimie de Clermont-Ferrand
Abstract : This PhD thesis is focused on studying enthalpy of solution of carbon dioxide in aqueous amine solutions. In order to develop theoretical models describing the {CO2-amine-water} systems under process conditions, reliable experimental data for solubility and enthalpy are required. In this study, we used a custom-made flow mixing unit in the SETARAM C-80 calorimeter to measure the enthalpy of solution of CO2 in five aqueous amine solutions (2-Amino-2-methyl-1-propanol (AMP), monoethanolamine (MEA), diethanolamine (DEA), triethanolamine (TEA) and methyldiethanolamine (MDEA)) (15 and 30 wt%) at temperatures between 322.5 K and 372.9 K and pressures from 0.5 to 5 MPa. Literature data were used to derive two VLE thermodynamic models (a simple one and a rigorous one). The first model treats the CO2 absorption by one single reaction, while the second takes into account all reactions occurring at equilibrium. The simple model reproduces our experimental enthalpies to within 10%, while the full chemical equilibrium treatment reproduced our data to within 5-20% depending on the amine selected. The enthalpy calculation in the rigorous model is strongly dependent of the literature values used for the amine protonation reaction. Accurate protonation constant measurements are needed to resolve this issue.
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Hugues Arcis. Etude thermodynamique de la dissolution du dioxyde de carbone dans des solutions aqueuses d'alcanolamines. Chimie organique. Université Blaise Pascal - Clermont-Ferrand II, 2008. Français. ⟨NNT : 2008CLF21901⟩. ⟨tel-00731443⟩

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