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Experimental Determination and Equation of State Modeling of High-Pressure Fluid Behavior

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Experimental Determination and Equation of State Modeling of High-Pressure Fluid Behavior Virginia Commonwealth University VCU Scholars Compass Theses and Dissertations Graduate School 2013 Experimental Determination and Equation of State Modeling of High-Pressure Fluid Behavior Yue Wu Virginia Commonwealth University Follow this and additional works at: https://scholarscompass.vcu.edu/etd Part of the Engineering Commons © The Author Downloaded from https://scholarscompass.vcu.edu/etd/3237 This Dissertation is brought to you for free and open access by the Graduate School at VCU Scholars Compass. It has been accepted for inclusion in Theses and Dissertations by an authorized administrator of VCU Scholars Compass. For more information, please contact [email protected]. Experimental Determination and Equation of State Modeling of High-Pressure Fluid Behavior A dissertation submitted in partial fulfillment of the requirements for the degree of Doctor of Philosophy at Virginia Commonwealth University. by Yue Wu, Doctor of Philosophy, Virginia Commonwealth University, 2013 Director: Mark A. McHugh, Professor, Department of Chemical and Life Science Engineering Virginia Commonwealth University Richmond, Virginia November, 2013 Acknowledgment I thank my advisor, Professor Mark A. McHugh for his support, encouragement, and guidance throughout this research over the years. He will always be given my respect for guiding me through the ocean of chemical engineering. His devotion to the science, great personality, and sense of humor impress me a lot. I do enjoy working in Professor McHugh’s Lab and I am very grateful to have such a great advisor. I appreciate my PhD committee members, Professor Everett Carpenter, Professor Stephen Fong, Professor Vamsi Yadavalli, and Professor Hu Yang for their time and efforts. I acknowledge Dr. Isaac Gamwo, Dr. Deepak Tapriyal, Professor Robert Enick, Dr. Ward Burgess, Dr. Hseen Baled for their continual support, valuable remarks, and helpful technical discussions. I express my gratitude to Mr. Matthew Newkirk, Mr. Babatunde Bamgbade, Mr. Sean Dudek, Dr. Rajendar R. Mallepally, and Mr. Michael Marin for their helpful discussions and exchange of ideas. I acknowledge National Energy Technology Laboratory and Afton Chemical Corporation for their financial support. I thank my family and girlfriend for their support throughout my life. I wish all of them health and happiness. ii Table of Contents List of Tables .................................................................................................................................. v List of Figures .............................................................................................................................. viii List of Abbreviations ..................................................................................................................... xi Abstract ........................................................................................................................................ xiv Chapter 1 Introduction .................................................................................................................... 1 1.1. High-Pressure Behavior of Low Molecular Weight Compounds ........................................ 2 1.1.1. Role of High-Pressure Solution Behavior in Industrial Applications ........................... 2 1.1.2. Experimental Techniques for High-pressure Density Determination ........................... 3 1.1.3. Literature Review of Available Data .......................................................................... 15 1.1.4. Low Molecular Compounds Investigated in This PhD Work .................................... 24 1.2. High-Pressure Solution Behavior of Highly Branched Polymer Solutions ....................... 25 1.2.1. Role of High-Pressure Polymer-SCF Solutions in Industrial Applications ................ 26 1.2.2. Effect of Branched Architecture on High-Pressure Solution Behavior ...................... 27 1.2.3. Solution Behavior Differences between Star and Linear Polymers in Liquid Solvents ............................................................................................................................................... 29 1.2.4. Polymer-Solvent Mixtures investigated in This PhD Work ....................................... 32 1.3. Modeling High-Pressure Solution Behavior ...................................................................... 32 1.3.1. Role of Cubic Equation of State (EoS) in Industrial Applications ............................. 34 1.3.2. Volume-Translated Cubic EoS ................................................................................... 36 1.3.3. Perturbed-Chain Statistical Associating Fluid Theory (PC-SAFT) ............................ 41 1.3.4. Copolymer PC-SAFT EoS .......................................................................................... 48 1.3.5. Summary of EoS Models ............................................................................................ 49 1.4. Objectives of This PhD Study ........................................................................................... 50 Chapter 2 Experimental Techniques ............................................................................................. 52 2.1. High-Pressure, Volume-Variable View Cell Apparatus .................................................... 52 2.1.1. Calibration of the Pressure Transducer and Thermocouple ........................................ 53 2.1.2. Calibration of Internal Cell Volume ........................................................................... 58 2.1.3. Density Determination ................................................................................................ 61 2.1.4. Cloud-Point Curve Determination .............................................................................. 62 2.1.5. Error Analysis ............................................................................................................. 63 2.2. High-Pressure Fractionation Apparatus and Technique .................................................... 64 Chapter 3 Solution Behavior and Modeling: Low Molecular Weight Compounds ..................... 66 3.1. High-Pressure Densities ..................................................................................................... 66 iii 3.1.1. Experimental Results .................................................................................................. 66 3.1.2. Comparisons with Available Literature Data ............................................................. 77 3.1.3. Isomer Structural Effects on High-Pressure Density .................................................. 87 3.2. Density Predictions ............................................................................................................ 89 3.2.1. Physical Properties and Parameters needed for EoS Modeling .................................. 89 3.2.2. Comparison of experimental data and model calculations ......................................... 92 3.2.3. Analysis of the Performance of PC-SAFT EoS Modeling ....................................... 103 3.2.4. EoS Performance for Capturing Structural Effect for Isomers ................................. 107 3.2.5. Optimization of PC-SAFT Pure-Component Parameters ......................................... 109 3.3. Final Comments ............................................................................................................... 115 Chapter 4 Solution Behavior and Modeling of Star Polymer Solutions ..................................... 116 4.1. Star Polymer Synthesis and Characterization .................................................................. 116 4.2. Fractionation .................................................................................................................... 118 4.3. Phase Behavior Determination in Supercritical Propane ................................................. 122 4.3.1. Homogeneous Polymer and Linear Copolymers ...................................................... 122 4.3.2. Star Polymer Fractions .............................................................................................. 125 4.3.3. Star Morphology Effects on Phase Behavior ............................................................ 127 4.4. Density Determination ..................................................................................................... 128 4.5. PC-SAFT EoS Modeling ................................................................................................. 131 4.5.1. Pure-Component Parameters .................................................................................... 131 4.5.2. Results and Discussions ............................................................................................ 132 4.6. Final Comments ............................................................................................................... 134 Chapter 5 Conclusions and Future Work .................................................................................... 135 5.1. Conclusions ...................................................................................................................... 135 5.2. Future Work ..................................................................................................................... 136 Bibliography ............................................................................................................................... 139 Vita .............................................................................................................................................
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