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Improving Thermodynamic Consistency Among Vapor Pressure, Heat of Vaporization, and Liquid and Ideal Gas Heat Capacities Joseph Wallace Hogge Brigham Young University

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Improving Thermodynamic Consistency Among Vapor Pressure, Heat of Vaporization, and Liquid and Ideal Gas Heat Capacities Joseph Wallace Hogge Brigham Young University Brigham Young University BYU ScholarsArchive All Theses and Dissertations 2017-12-01 Improving Thermodynamic Consistency Among Vapor Pressure, Heat of Vaporization, and Liquid and Ideal Gas Heat Capacities Joseph Wallace Hogge Brigham Young University Follow this and additional works at: https://scholarsarchive.byu.edu/etd Part of the Chemical Engineering Commons BYU ScholarsArchive Citation Hogge, Joseph Wallace, "Improving Thermodynamic Consistency Among Vapor Pressure, Heat of Vaporization, and Liquid and Ideal Gas Heat Capacities" (2017). All Theses and Dissertations. 6634. https://scholarsarchive.byu.edu/etd/6634 This Dissertation is brought to you for free and open access by BYU ScholarsArchive. It has been accepted for inclusion in All Theses and Dissertations by an authorized administrator of BYU ScholarsArchive. For more information, please contact [email protected], [email protected]. Improving Thermodynamic Consistency Among Vapor Pressure, Heat of Vaporization, and Liquid and Ideal Gas Heat Capacities Joseph Wallace Hogge A dissertation submitted to the faculty of Brigham Young University In partial fulfillment of the requirements for the degree of Doctor of Philosophy W. Vincent Wilding, Chair Thomas A. Knotts Dean Wheeler Thomas H. Fletcher John D. Hedengren Department of Chemical Engineering Brigham Young University Copyright © 2017 Joseph Wallace Hogge All Rights Reserved ABSTRACT Improving Thermodynamic Consistency Among Vapor Pressure, Heat of Vaporization, and Liquid and Ideal Gas Heat Capacity Joseph Wallace Hogge Department of Chemical Engineering, BYU Doctor of Philosophy Vapor pressure ( ), heat of vaporization ( ), liquid heat capacity ( ), and ideal gas heat capacity ( ) are important properties for process design and optimization. This work vap Δvap focuses on improving the thermodynamic consistency and accuracy of the aforementioned properties since these can drastically affect the reliability, safety, and profitability of chemical processes. They can be measured for pure organic compounds from the triple point, through the normal boiling point, and up to the critical point. Additionally, is proportional to the derivative of vapor pressure with respect to temperature through the Clapeyron equation, and the vap difference between and is proportional to the derivative Δof heat of vaporization with respect to temperature. In order to improve temperature-dependent correlations, all the properties were analyzed simultaneously. First, a temperature-dependent error model was developed using several versions of the Riedel and Wagner correlations. The ability of each correlation to match data was determined for 5 well-known compounds. The Riedel equation performed better than the Wagner vap equation when the best form was used. Second, the Riedel equation form was further modified, and the best correlation form was found for about 50 compounds over 7 families. This led to the development of a new vapor pressure prediction method using different Riedel equation forms to fit , , and data simultaneously. Seventy compounds were tested, and the error compared to liquid heat capacity data dropped from 10% with previous methods to 3% with this vap vap new predictionΔ method. Additionally a differential scanning calorimeter (DSC) was purchased, and melting points ( ), enthalpies of fusion ( ), and liquid heat capacities ( ) were measured for over twenty compounds. For many of these compounds, the vapor pressure data and critical constants were fus re-evaluated, and new vaporΔ pressure correlations were recommended that were thermodynamically consistent with measured liquid heat capacity data. The Design Institute for Physical Properties (DIPPR) recommends best constants and temperature-dependent values for pure compounds. These improvements were added to DIPPR procedures, and over 200 compounds were re-analyzed so that the temperature-dependent correlations for , , , and became more internally consistent. Recommendations were made for the calculation procedures of these properties for the DIPPR database. vap vap Δ Keywords: multi-property optimization, vapor pressure, heat capacity, heat of vaporization ACKNOWLEDGEMENTS I would like to thank all of the people who helped me in this project and made it possible. I thank my wife, Julie, and our 2 kids, Louisa and Adelaide, for all of their unwavering support and motivation. My gratitude goes out to my advisor, Dr. Wilding, along with Dr. Knotts, Dr. Giles, and other members of my committee that helped bring this project to fruition. I would also like to thank my father, Jeff, who talked me through my freshman writing class. Without his encouragement, I would never have thought it possible to write this document. I thank my mother, Kim, for instilling in me a desire to learn about the world around us. TABLE OF CONTENTS LIST OF TABLES ....................................................................................................................... viii LIST OF FIGURES ..................................................................................................................... xvi 1 Introduction ............................................................................................................................. 1 2 Thermodynamic Relationships ................................................................................................ 4 3 Literature Review of Thermophysical Properties .................................................................... 7 3.1 Vapor Pressure ................................................................................................................. 7 3.1.1 Vapor Pressure Correlation Equations ............................................................. 7 3.1.2 Vapor Pressure Data Availability .................................................................... 9 3.2 Heat of Vaporization ........................................................................................................ 9 3.2.1 Heat of Vaporization Correlation Equations .................................................. 10 3.2.2 Heat of Vaporization Data Availability ......................................................... 10 3.3 Ideal Gas Heat Capacity ................................................................................................. 12 3.3.1 Ideal Gas Heat Capacity Correlation Equations ............................................ 12 3.3.2 Ideal Gas Heat Capacity Data Availability .................................................... 13 3.4 Liquid Heat Capacity ..................................................................................................... 17 3.4.1 Liquid Heat Capacity Temperature Behavior ................................................ 18 3.4.2 Liquid Heat Capacity Data Availability ........................................................ 20 3.5 Analysis of Experimental Data and Correlations ........................................................... 20 4 Multi-Property Optimization – Temperature Dependent Errors ........................................... 23 4.1 Weight Model ................................................................................................................. 23 4.2 Results/Discussion ......................................................................................................... 25 4.3 Conclusions .................................................................................................................... 29 5 Multi-Property Optimization – The Riedel Equation ............................................................ 31 5.1 Methods .......................................................................................................................... 31 5.2 Results ............................................................................................................................ 34 5.3 Conclusions .................................................................................................................... 44 6 New Thermodynamically Consistent Vapor Pressure Prediction ......................................... 46 6.1 Introduction .................................................................................................................... 47 iv 6.2 Overview of Vapor Pressure Prediction and Correlation Methods ................................ 48 6.3 Theory ............................................................................................................................ 51 6.3.1 Thermodynamic Relationships ...................................................................... 51 6.3.1 New Predictive Vapor Pressure Method ........................................................ 51 6.4 Methods .......................................................................................................................... 53 6.4.1 Regression of K and Xc as a Function of E .................................................... 53 6.4.2 E Training Method ......................................................................................... 56 6.5 Results ............................................................................................................................ 57 6.5.1 Optimized E by Family .................................................................................. 57 6.5.2 Comparison to Other Predictive Methods...................................................... 60 6.5.3 Testing the Methods with Compounds Not Used in the Training Set ........... 63 6.6 Conclusions ...................................................................................................................
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