Experimental measurements and modelling of the dissociation conditions of gas semi-clathrate hydrates formed with TBAB, TBAC, TBAF, and TBPB salts

Abstract : Semiclathrate hydrates can entrap gas molecules (e.g. CO2, H2, CH4, and N2) and can form at atmospheric pressure and near ambient temperatures. Therefore, semiclathrate hydrates have been extensively studied for applications such as gas capture and storage, gas mixture separation, and refrigeration. In this study, we experimentally and theoretically investigate the dissociation condition for gas semiclathrate hydrates formed with alkyl-substituted quaternary ammonium salts on the purpose of H2 storage and H2+CO2 gas mixture separation. Paricaud (2011) [1] proposed a model to determine the formation conditions of gas semiclathrates hydrates and determined parameters for CO2+ tetra-n-butyl ammonium bromide (TBAB) + water system. The aim of this study is to extend the model to other semiclathrate hydrate systems. Since there are many experimental data for CO2+ tetra-n-alkyl ammonium salts +water system, we have first modeled CO2 semiclathrate hydrates with the following salts: tetra-n-butyl ammonium fluoride (TBAF), tetra-n-butyl ammonium chloride (TBAC), and tetra-n-butyl phosphonium bromide (TBPB). Good predictions were obtained over a wide range of concentrations of the salts: 0.03≤wTBAB≤0.55, 0.04≤wTBAC≤0.34, 0.02≤wTBAF≤0.448, 0.05≤wTBPB≤0.6 and pressure up to 5 MPa. Some experimental data for H2+ tetra-n-alkyl ammonium salts +water systems have been reported in the literature [2], but such data are still scare. Therefore we have conducted experimental measurements of the dissociation temperatures for TBAC semiclathrate hydrates in the presence of H2 using pressure-controlled differential scanning calorimetry. Measurements were conducted at wTBAC = 0.10, 0.20, 0.35, and 0.50 in pressure range up to 15.5 MPa. The amount of hydrogen stored in the semiclathrate hydrate was estimated to be 0.43 wt% at 289.75 K and 15.5 MPa.
Type de document :
Communication dans un congrès
8th International Conference on Gas Hydrates, Jul 2014, Beijing, China. pp.1
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Contributeur : Didier Dalmazzone <>
Soumis le : jeudi 23 juillet 2015 - 13:41:02
Dernière modification le : jeudi 16 novembre 2017 - 17:14:19

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  • HAL Id : hal-01179808, version 1

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Didier Dalmazzone, Patrice Paricaud, Ayako Fukumoto. Experimental measurements and modelling of the dissociation conditions of gas semi-clathrate hydrates formed with TBAB, TBAC, TBAF, and TBPB salts. 8th International Conference on Gas Hydrates, Jul 2014, Beijing, China. pp.1. 〈hal-01179808〉

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