HIGH-PRESSURE/HIGH-TEMPERATURE GAS-SOLUBILITY STUDY IN HYDROGEN-PHENANTHRENE AND METHANE-PHENANTHRENE SYSTEMS USING STATIC AND CHROMATOGRAPHIC TECHNIQUES

[摘要] The design and discovery of sources for alternative energy such as coal liquefaction has become of major importance over the past two decades. One of the major problems in such design is the lack of available data, particularly, for gas solubility in polycyclic aromatics at high temperature and pressure. Static and gas-liquid partition chromatographic methods were used for the study of hydrogen-phenanthrene and methane-phenanthrene systems. The static data for these two binaries were taken along 398.2, 423.2, 448.2, 473.2 K isotherms up to 25.23 MPa. Pressure versus liquid mole fraction plots were presented as well as linear ln(f$sbsp{m i}{hinspacem g}$/x$sb{m i}$) versus P-P$sbsp{m s}{m vap}$ graphs. Using estimates of the partial molar volume in the liquid phase, V$sbsp{m i}{infty}$, the latter plots indicated both pressure and small liquid mole fraction deviations from ideal solution. Gas-liquid partition chromatography was used to study the infinite dilution behavior of methane, ethane, propane, n-butane, and carbon dioxide in the hydrogen-phenanthrene system as well as hydrogen, ethane, n-butane, and carbon dioxide in the methane-phenanthrene binary. The principle objective was to examine the role of the elution gas. Temperatures were along the same isotherms as the static data and up to 20.77 MPa. Comparison of the hydrogen and methane elution gas results indicated that the PK$sbsp{m i}{infty}$ product increases much more rapidly with pressure for the methane carrier data. However, plots of ln(PK$sbsp{m i}{infty}phisbsp{m i}{infty}$) versus P-P$sbsp{m s}{m vap}$ were the same in both elution gases for ethane and n-butane. Using V$sbsp{m i}{infty}$ estimates, the plots displayed deviations from ideal solution due to pressure effects alone, with carrier gas absorption having essentially no effect. This was contrary to previous conclusions for infinitely dilute data in the hydrogen-9-methylanthracene system. Analysis of this data also indicated hydrogen solubility was not important. With the exception of carbon dioxide, Henry;;s constants were calculated for all systems. Expressions for the heat of solution as a function of pressure were derived for both binary and chromatographic data. Estimates of $Delta$H$sbsp{m i}{m sol}$ at high pressure were presented.

[发布机构] Rice University