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Journal Articles Journal of Physical Chemistry B Year : 2004

Thermodynamic and dynamic interfacial properties of binary carbon dioxide-water systems

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Abstract

We have measured the interfacial tension (γ) between H2O and CO2 with a drop tensiometer that permitted us to regulate the drop area and to perform elasticity measurements. We observed that γ decreased with time and with the CO2 pressure. We first analyzed the adsorption of CO2 onto surface water by plotting the initial interfacial tension (γ0) versus CO2 fugacity and applied Gibbs and then Langmuir-Freundlich equations. We have calculated the interfacial area occupied by CO2 onto H2O as well as the equilibrium constant and the thermodynamics parameters of adsorption. This permitted us to understand that the CO2 was adsorbed onto the surface water by formation of a one-to-one H-type complex with H2O. Second, we attributed the kinetics phenomena to the formation of interfacial clusters between water and CO2, which gave interfacial quasi-crystalline structure as shown by compression of the drop area at the end of the adsorption kinetics. We studied this interfacial organization by measuring the apparent elasticity versus time and CO2 pressure. This measurement allowed us to propose an interfacial organization based on the formation of small blocks, which grow to fill the interface, as already observed by Teng and al. Then we determined the filling of the clusters cavities by analyzing the difference between γ0 and γeq (Δγ) by means of the Hill equation. This permitted us to determine that this filling depended on temperature and was cooperative
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Dates and versions

inserm-00264730 , version 1 (17-03-2008)

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Frédéric Tewes, Frank Boury. Thermodynamic and dynamic interfacial properties of binary carbon dioxide-water systems. Journal of Physical Chemistry B, 2004, 108 (7), pp.2405-2412. ⟨10.1021/jp030895c⟩. ⟨inserm-00264730⟩

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