International audienceIn this paper, a set of experimental data on the phase equilibrium of gas hydrates in the presence of binary gas mixtures comprising CO2 is presented. The procedure established allows for the determination of both the composition of the gas phase as well as the hydrate phase without the need to sample the hydrate. The experimental results obtained in these measurements have been described by means of the classical model of van der Waals and Platteeuw. The values of internal parameters of the reference state and the Kihara parameters have been re-discussed and their interdependency is pointed. Finally the new set of parameters is validated against experimental data from other sources available in the literature, or invalidated against other sources. Finally, we conclude on the difference of experimental data between laboratories. The differences are not on the classical (pressure, temperature, gas composition) data which appear equivalent between laboratories. The difference stands on the measurement composition of the hydrate phase
Re´sume´-Ame´lioration de la se´lectivite´du captage du CO 2 dans les semi-clathrates hydrates en utilisant les ammoniums quaternaires comme promoteurs thermodynamiques -La re´duction des e´missions de CO 2 est tre`s probablement l'un des enjeux importants de ce sie`cle. La capture puis le stockage ge´ologique de ce gaz, a`partir de sources industrielles ponctuelles et massives, est une voie d'importance. L'une des voies technologiques consiste a`utiliser les clathrates hydrates, ou semi-clathrates hydrates, qui ne´cessitent de pressuriser le gaz en amont du proce´de´. Sous pression, l'eau et les gaz forment un solide qui encapsule pre´fe´rentiellement le CO 2 , puis le gaz peut-eˆtre ensuite re´cupe´re´sous pression apre`s la dissociation du solide. L'abaissement de la pression ope´ratoire est un objectif en soi afin de faire baisser les couˆts ope´ratoires. Cet abaissement peut eˆtre obtenu par l'utilisation de promoteurs thermodynamiques, dont les sels d'ammonium quaternaires constituent une famille inte´ressante puisqu'ils forment des solides naturellement anti-agglome´rants, et plus facilement manipulables. Dans ce travail, nous pre´sentons de nouveaux re´sultats expe´rimentaux sur les e´quilibres des semi-clathrates de (CO 2 , N 2 ) en pre´sence de Tetra-n-Butyl Ammonium Bromide (TBAB). Nous donnons des mesures expe´rimentales de pression et tempe´rature en fonction de la concentration en TBAB. La pression ope´ratoire peut eˆtre abaisse´e jusqu'a`la pression atmosphe´rique. Nous donnons aussi une information supple´mentaire portant sur la composition de l'hydrate. Nous observons que la se´lectivite´du CO 2 dans les semi-clathrates hydrates est bien meilleure que pour les clathrates hydrates traditionnels, sans promoteur thermodynamique.Abstract -Enhanced Selectivity of the Separation of CO 2 from N 2 during Crystallization of SemiClathrates from Quaternary Ammonium Solutions -CO 2 mitigation is crucial environmental problem and a societal challenge for this century. CO 2 capture and sequestration is a route to solve a part of the problem, especially for the industries in which the gases to be treated are well localized. CO 2 capture by using hydrate is a process in which the cost of the separation is due to compression of gases to reach the gas hydrate formation conditions. Under pressure, the water and gas form a solid that encapsulates preferentially CO 2 . The gas hydrate formation requires high pressures and low
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