The solubility of solutes in cryogenic liquids

Wu, Ming Fai (1986) The solubility of solutes in cryogenic liquids. University of Southampton, Doctoral Thesis.

Abstract

The solubilities of carbon dioxide, nitrous oxide, water, hydrogen sulphide, methanol, ethanol and some aliphatic ethers have been experimentally measured in cryogenic liquids between 77 and 135K using infrared spectroscopy in a specially constructed high pressure (up to 30 bar) infrared absorption cell. The design of the high pressure cell and the experimental procedures have been described in detail. Compounds such as carbon dioxide, nitrous oxide and aliphatic ethers have been found to be considerably soluble in cryogenic liquids with solubilities ranging from 10^-8 to 10^-4 mole fraction. The solubility data have been measured as a function of temperature and the enthalpies of solution have been determined from the slopes of the linear solubility curves. The solubilities of water, hydrogen sulphide, methanol and ethanol have been experimentally found to be very low i.e. less than 10¹⁰ mole fraction in liquid nitrogen (77K), liquid oxygen (90K) and liquid argon (87K) mainly because of the strong hydrogen bonding interactions between the solute molecules. These values are considerably lower than those measured previously using gravimetric methods (10^-7 to 10^-5 mole fraction). A number of criteria for assessing the solubilities of solutes in cryogenic liquids are therefore proposed to avoid controversies and experimental artefacts. The experimental solubilities are compared with the predicted values based on the Ideal and Regular Solution theories. Both theories have failed to predict the solubilities comparable to the experimental values. A simple model for predicting the solubility of a solute in multi-component systems using the binary solubility data obtained in this work is proposed. (D72200/87)

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