Phase equilibrium data for semiclathrate hydrates formed with n-propyl, tri-n-butylammonium bromide and tri-n-butyl, n-pentylammonium bromide under methane, carbon dioxide and nitrogen gas pressure

Abstract

Semiclathrate hydrates are water-based materials formed from aqueous solutions of ionic substances. To enhance the gas capture performance of these materials, it is necessary to direct focus on the cation, which is a key part of construction of the hydrogen-bonding framework. In this paper, we focus on the partly-asymmetric cations, i.e., the n-propyl, tri-n-butylammonium bromide (N3444Br) and tri-n‑butyl, n-pentylammonium bromide (N4445Br), which are yet to be subjected to gas hydrate formation. The three phase equilibrium (gas–hydrate–liquid) conditions for the systems of (N3444Br or N4445Br) + H₂O + (CH₄, CO₂ or N₂) in the range of the pressure and mass fractions of the aqueous solutions between 1 and 11 MPa and 0.10–0.40, respectively, are reported. In all the systems, the semiclathrate hydrates were successfully formed under gas pressure. It was demonstrated that both the N3444Br and N4445Br salts promoted hydrate formation under these gases, while in the case with lean aqueous solutions N3444Br acted as an inhibitor of methane hydrate formation in pure water system. The present data are compared with the literature data, and the effect of the side chain length on the phase behavior of the semiclathrate hydrate phase is discussed.