Experimental study of impurity freeze-out in ternary methane + ethane + benzene mixtures with applications to LNG production

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The freeze-out of impurities in LNG production can pose significant operational risks and lead to costly blockage-induced plant shutdowns. Study of ternary and higher-order mixtures, which are more analogous to LNG, present the critical tests of thermodynamic models in terms of their utility and predictive accuracy. In this work, a visual CryoSolids apparatus was upgraded to allow analytical measurements of solvent composition in multi-component systems where a solid phase is present at equilibrium. The analytical system, which included a ROLSI sampling valve and capillary together with a gas chromatograph, was successfully commissioned and used to measure melting temperatures and solvent compositions of a ternary mixture containing methane, ethane, and benzene at temperatures down to 125 K and pressures up to 6 MPa. The effect on the solubility of benzene by adding ethane to the solvent was investigated by varying the ethane mole fraction from 0 to 0.96. The resulting temperature at which benzene melted into the liquid solvent decreased from 246 K at 4.7 MPa to 125 K at 5.7 MPa. The comparison of results with the ThermoFAST model showed that it could describe the new data with a deviation less than 1 K for ethane liquid phase mole fractions from 0 < xC2< 0.5, which increased to less than 4 K for 0.85 < xC2< 0.97. This result indicates that ThermoFAST satisfactorily represents SFE conditions in LNG mixtures of industrial relevance but needs improvement to cover wider ranges of composition.

Original languageEnglish
Article number103918
JournalJournal of Natural Gas Science and Engineering
Publication statusPublished - Jun 2021


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