Phase equilibrium measurements and modelling for separation process design

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School of Chemical Technology | Doctoral thesis (article-based) | Defence date: 2012-03-16
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Date
2012
Major/Subject
Mcode
Degree programme
Language
en
Pages
128
Series
Aalto University publication series DOCTORAL DISSERTATIONS, 20/2012
Abstract
The purpose of this research was to develop modelling of industrial processes by improving the thermodynamic representation of the equilibrium between phases. For this purpose an extensive experimental work was performed, comprising of vapour-liquid, gas-liquid and solid-liquid equilibrium measurements. Vapour liquid equilibrium of binary mixtures of butane + alcohols was measured with a static total pressure apparatus due to the importance of hydrocarbon and alcohol mixtures in the production of biofuels. The same equipment was used to measure binary systems of diethyl sulphide + C4 - hydrocarbons of importance in refinery applications. The activity coefficients of these systems were modelled with activity coefficients models. The absorption of carbon dioxide in alkanolamine solutions is the leading technology for the removal of carbon dioxide during refining of gas and oil. In recent years, this technology has gained importance also for carbon capture from large point sources. The scarcity of experimental data for some alkanolamine systems affected the accuracy of thermodynamic models. Several experimental techniques were developed to supply new experimental data for aqueous solutions of diisopropanolamine (DIPA) and methyldiethanolamine (MDEA). The solubility of carbon dioxide in solutions of these amines was measured with a static total pressure apparatus for gas solubility, and with a bubbling apparatus. The density of carbonated aqueous DIPA was also measured and modelled. The vapour-liquid equilibrium of water + DIPA and water + MDEA was measured with a static total pressure apparatus. The solid-liquid equilibrium of the same systems was measured with a visual method and a Differential Scanning Calorimeter. The activity coefficients of aqueous DIPA and MDEA solutions were modelled using NRTL, thus providing the first model of this sort for DIPA. A new model of the Henry's law constant of carbon dioxide in binary and ternary aqueous solutions of alkanolamines was developed at temperatures up to 393 K.
Description
Supervising professor
Alopaeus, Ville, Professor
Thesis advisor
Aittamaa, Juhani, Dr.
Keywords
vapour-liquid equilibrium, solid-liquid equilibrium, solubility, carbon dioxide, diisopropanolamine, methyldiethanolamine, butane, diethyl sulphide, UNIFAC, COSMO, Henry's law, miniplant
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Parts
  • [Publication 1]: Anne Penttilä, Claudia Dell'Era, Petri Uusi-Kyyny, and Ville Alopaeus. 2011. The Henry's law constant of N2O and CO2 in aqueous binary and ternary amine solutions (MEA, DEA, DIPA, MDEA, and AMP). Fluid Phase Equilibria, volume 311, pages 59-66.
  • [Publication 2]: Claudia Dell'Era, Petri Uusi-Kyyny, Eeva-Leena Rautama, Minna Pakkanen, and Ville Alopaeus. 2010. Thermodynamics of aqueous solutions of methyldiethanolamine and diisopropanolamine. Fluid Phase Equilibria, volume 299, number 1, pages 51-59.
  • [Publication 3]: Claudia Dell'Era, Petri Uusi-Kyyny, Juha-Pekka Pokki, Minna Pakkanen, and Ville Alopaeus. 2010. Solubility of carbon dioxide in aqueous solutions of diisopropanolamine and methyldiethanolamine. Fluid Phase Equilibria, volume 293, number 1, pages 101-109.
  • [Publication 4]: Claudia Dell'Era, Juha-Pekka Pokki, Petri Uusi-Kyyny, Minna Pakkanen, and Ville Alopaeus. 2010. Vapour-liquid equilibrium for the systems diethyl sulphide + 1-butene, +cis-2-butene, +2-methylpropane, +2-methylpropene, +n-butane, +trans-2-butene. Fluid Phase Equilibria, volume 291, number 2, pages 180-187.
  • [Publication 5]: Claudia Dell'Era, Anna Zaytseva, Petri Uusi-Kyyny, Juha-Pekka Pokki, Minna Pakkanen, and Juhani Aittamaa. 2007. Vapour-liquid equilibrium for the systems butane + methanol, +2-propanol, +1-butanol, +2-butanol, +2-methyl-2-propanol at 364.5 K. Fluid Phase Equilibria, volume 254, numbers 1-2, pages 49-59.
  • [Publication 6]: Tuomas Ouni, Petri Lievo, Petri Uusi-Kyyny, Claudia Dell'Era, Kaj Jakobsson, Antti Pyhälahti, and Juhani Aittamaa. 2006. Practical methodology for distillation design using a miniplant. Chemical Engineering & Technology, volume 29, number 1, pages 104-112.
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