This paper presents the three-phase (liquid−hydrate−vapor) equilibrium conditions for the binary and ternary systems constituted by methane (CH 4 ) or ethane (C 2 H 6 ) + tetra-n-butylphosphonium bromide (TBPB, C 16 H 36 BrP) + water (H 2 O). The experiments were carried using the isochoric method within the temperature and pressure ranges of (277.0−293.5) K and (0.65−9.22) MPa, respectively. Phase equilibria for binary systems, CH 4 + H 2 O and C 2 H 6 + H 2 O, were in good agreement when they were compared with previously reported data. Different mass fractions of aqueous TBPB solutions (w TBPB ) in the range of (0.0099−0.20) were studied. For the ternary CH 4 + C 16 H 36 BrP + H 2 O system, it was observed that the ionic liquid has promotional effects for the gas hydrate formation in the range of w TBPB = 0.05−0.20 since the three-phase equilibrium curves moved toward low-pressure and high-temperature conditions, which agrees with previous results reported in the literature. From comparison, deviations are within the experimental errors. On the other hand, encouraging results were found only at w TBPB = 0.05 for the C 2 H 6 + C 16 H 36 BrP + H 2 O system, since the ionic liquid exhibited promotional effects; meanwhile, this effect decreased for w TBPB = 0.10 and 0.20, since the liquid−hydrate−vapor equilibrium curves were closer to that of ethane hydrate, and under some conditions (w TBPB = 0.20), the ionic liquid had suppressing capabilities where the equilibrium curve moved to temperatures lower than the corresponding ethane hydrate. Standard uncertainties of temperature and pressure in the three-phase equilibrium measurements were estimated to be u(T) = 0.13 K and u(p) = 0.07 MPa, respectively.
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