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The work reported here represents part of a long-term research objective of determining accurate experimental liquid-vapor phase equilibrium data on binary fluid mixtures in the temperature range 13-160 Kelvin and at pressures up to 4000 atm. Systems under investigation are those in which, under these conditions, one component is normally a gas and the other is a liquid. These substances are among those with the lowest critical temperatures and the simplest molecular structures. The gas-liquid critical curve extending into pressure-temperature-composition (PTX) space, from the critical point of argon, has been well-defined by eleven experimental points. It was found to pass through a minimum in temperature at 147.1K, and a pressure of 440 atm. These results confirm the presence of fluid-fluid equilibrium in this system at temperatures above the critical temperature of argon (150.86K). Additionally, the three phase boundary solid-liquid-gas (solid-fluid-fluid) has been determined at pressures to 4000 atm. (Author).
The high pressure phase behaviour of binary fluid mixtures has been extensively studied during the last three decades. There is ample experimental data for a wide variety of binary mixtures and extensive methods for prediction have been developed. In contrast, the investigation of ternary and other multicomponent fluids is in its infancy. Experimental ternary mixture critical data are very rare and theoretical studies have been limited to data correlation rather than genuine prediction. The phase behaviour of ternary and other multicomponent fluid mixtures has many novel aspects which are not manifested in binary mixtures. The properties of ternary mixtures are also likely to be more difficult to characterize experimentally. It is in this context that calculated phase diagrams have an important role in leading the discovery of new phenomena and guiding experimental work. The criteria for phase equilibria of multicomponent fluids with particular emphasis on the critical state are examined in this book, and models for predicting fluid equilibria (e.g., different equations of state) are compared. Particular attention is paid to the critical state of ternary mixtures which has hitherto been largely neglected. The problems associated with predicting ternary equilibria are discussed, and some novel aspects of ternary critical phenomena are illustrated. The books also describes a novel type of critical transition which appears to be a common feature of the equilibria of ternary mixtures. Extensive phase diagrams of a wide range of ternary mixtures including systems containing carbon dioxide, water, nitrogen and tetrafluoromethane as one or more component are presented. The theoretical treatment is detailed in the appendix and a computation of known experimental critical points is also included.
Phase Equilibrium in Mixtures deals with phase equilibrium and the methods of correlating, checking, and predicting phase data. Topics covered range from latent heat and vapor pressure to dilute solutions, ideal and near-ideal solutions, and consistency tests. Molecular considerations and their use for the prediction and correlation of data are also discussed. Comprised of nine chapters, this volume begins with an introduction to the role of thermodynamics and the criteria for equilibrium between phases, along with fugacity and the thermodynamic functions of mixing. The discussion then turns to some of the phase phenomena which may be encountered in chemical engineering practice; methods of correlating and extending vapor pressure data and practical techniques for calculating latent heats from these data; the behavior of dilute solutions both at low and high pressures for reacting and non-reacting systems; and the behavior of ideal and near-ideal solutions. The remaining chapters explore non-ideal solutions at normal pressures; practical methods for testing the thermodynamic consistency of phase data; and the extent to which the broad aspects of phase behavior may be interpreted in the light of simple molecular considerations. This book is intended primarily for graduate chemical engineers but should also be of interest to those graduates in physics or chemistry who need to use phase equilibrium data.
The book begins with an overview of the phase diagrams of fluid mixtures (fluid = liquid, gas, or supercritical state), which can show an astonishing variety when elevated pressures are taken into account; phenomena like retrograde condensation (single and double) and azeotropy (normal and double) are discussed. It then gives an introduction into the relevant thermodynamic equations for fluid mixtures, including some that are rarely found in modern textbooks, and shows how they can they be used to compute phase diagrams and related properties. This chapter gives a consistent and axiomatic approach to fluid thermodynamics; it avoids using activity coefficients. Further chapters are dedicated to solid-fluid phase equilibria and global phase diagrams (systematic search for phase diagram classes). The appendix contains numerical algorithms needed for the computations. The book thus enables the reader to create or improve computer programs for the calculation of fluid phase diagrams. introduces phase diagram classes, how to recognize them and identify their characteristic features presents rational nomenclature of binary fluid phase diagrams includes problems and solutions for self-testing, exercises or seminars
Phase Behavior provides the reader with the tools needed to solve problems requiring a description of phase behavior and specific pressure/volume/temperature (PVT) properties.
High-pressure solution behavior such as density and phase behavior is a critical fundamental property for the design and optimization of various chemical processes, such as distillation and extraction in the production and purification of oils, polymers, and other natural materials. In this Ph. D. study, solution behavior data are experimentally determined and equation of state (EoS) modeled for n-hexadecane, n-octadecane, n-eicosane, methylcyclohexane, ethylcyclohexane, cis-1,2-dimethylcyclohexane, cis-1,4-dimethylcyclohexane, trans-1,4-dimethylcyclohexane, o-xylene, m-xylene, p-xylene, and 2-methylnaphthalene at temperatures to 525 K and pressures to 275 MPa. A variable-volume view cell coupled with a linear variable differential transformer is used for the high-pressure determination. The reported density data are less than 0.4% of available literature data, which is within the estimated accumulated experimental uncertainty, 0.75%. Special attention is paid to the effect of architectural differences on the resultant high-pressure solution behavior. The reported data of low molecular weight hydrocarbons are modeled with Peng-Robinson (PR) equation of state (EoS), high-temperature high-pressure volume-translated cubic (HTHP VT-cubic) EoS, and perturbed-chain statistical fluid theory (PC-SAFT) EoS. The three pure-component parameters in PC-SAFT EoS can be either obtained from literature or from a group contribution (GC) method. Generally, PR EoS gives the worst predictions and HTHP VT-cubic EoS provides modest improvements over the PR EoS, but both of the equations underpredict the densities at high pressures. On the other hand, PC-SAFT EoS, with parameters from the literature or from a GC method, gives the improved density predictions with respect to PR EoS and HTHP VT-cubic EoS, although an overprediction of densities is found at high pressures. Model calculations also highlight the capability of these equations to account for the different densities observed for the hydrocarbon isomers. However, none of the EoS investigated in this study can fully account for the effect of isomeric structural differences on the high-pressure densities. For a better prediction of densities at high pressures, a new set of PC-SAFT pure-component parameters are obtained from a fit of the experimental density data obtained in this study and the mean absolution percent deviation is within 0.4%. The experimental technique and PC-SAFT EoS modeling method are extended to a star polymer-propane mixture. Star polymers with a fixed number of arms have a globular structure that does not promote chain entanglements. Star polymers can be synthesized with a large number of functional groups that can be readily modified to adjust their physical properties for specific applications in the areas of catalysis, coatings, lubrication, and drug delivery. In this study, a star polymer with a divinylbenzene core and statistically random methacrylate copolymer arms is synthesized with reversible addition-fragmentation-transfer method and fractionated with supercritical carbon dioxide and propane to obtain fractions with low molecular weight polydispersity. The phase behavior and density behavior are experimentally determined in supercritical propane for fractionated star polymers and the corresponding linear copolymer arms at temperatures to 423 K and pressures to 210 MPa. Experimental data are presented on the impact of the molecular weight, the backbone composition of the lauryl and methylmethacrylate repeat units in the copolymer arms, and the DVB core on the polymer-propane solution behavior. The star polymer is significantly more soluble due to its unique structure compared with the solubility of the linear copolymer arms in propane. The resultant phase behavior for the two homopolymers and the copolymers in propane are modeled using the PC-SAFT and copolymer PC-SAFT EoS, which give reasonable predictions for both phase behavior and density behavior. Model calculations are not presented for the phase behavior of the star polymers in propane since the PC-SAFT approach is not applicable for star polymer structures.
Developed in conjunction with several oil companies using experimental data for real reservoir fluids, Phase Behavior of Petroleum Reservoir Fluids introduces industry standard methods for modeling the phase behavior of petroleum reservoir fluids at different stages in the process. Keeping mathematics to a minimum, this book discusses sampling, cha