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Supercritical Water Gasification of Two-Carbon Carboxylic Acid Derivatives

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Supercritical Water Gasification of Two-Carbon Carboxylic Acid Derivatives Supercritical Water Gasification of Two-Carbon Carboxylic Acid Derivatives A thesis presented to the faculty of the Russ College of Engineering and Technology of Ohio University In partial fulfillment of the requirements for the degree Master of Science Matthew T. Conley December 2018 © 2018 Matthew T. Conley. All Rights Reserved. 2 This thesis titled Supercritical Water Gasification of Two-Carbon Carboxylic Acid Derivatives by MATTHEW T. CONLEY has been approved for the Department of Chemical and Biomolecular Engineering and the Russ College of Engineering and Technology by Sunggyu Lee Professor, Chemical and Biomolecular Engineering Dennis Irwin Dean, Russ College of Engineering and Technology 3 ABSTRACT CONLEY, MATTHEW T., M.S., December 2018, Chemical Engineering Supercritical Water Gasification of Two-Carbon Carboxylic Acid Derivatives Director of Thesis: Sunggyu Lee The dominant means of energy production today consist of the use of nonrenewable and environmentally harmful fossils that cannot be used for eternity. Alternative energy sources are needed to combat the use of these fossil fuels and to one day replace them altogether. One potential fuel source is synthesis gas that can be derived from biomass and biomass waste. A production method for this synthesis gas is in the form of supercritical water gasification (SCWG). While SCWG is a relatively well- known process on a macro-level, little is known about the process at a molecular level. This work focuses on the study of the SCWG of three different two-carbon carboxylic acid derivatives – acetaldehyde, acetic acid, and acetamide – to get a better understanding of the gasification process itself. SCWG reactions were run on the three feedstocks in a custom built, high nickel alloy reactor at temperatures of 650 °C and 3600 psi with a residence time of 30 seconds. Gaseous products were quantified and analyzed via gas chromatography to determine reaction parameters such as composition, yield, and gasification rate. Acetaldehyde had hydrogen yields of about 1.1 to 1.7 moles H2 per mole acetaldehyde fed while acetic acid and acetamide had yields of around 0.02 moles H2 per mole reactant. It was determined that the process of SCWG of carbonyl groups seemingly follows the same reactivity trend as that of general nucleophilic attack of carbonyls, which makes it likely that the SCWG of carbonyls occurs via the nucleophilic attack of water towards these carbonyl groups. 4 DEDICATION To my family, whose support through the years has made me the person I am today and has allowed for me to finish this work. 5 ACKNOWLEDGMENTS First, I would like to express my gratitude towards my advisor, Dr. Sunggyu Lee, whose guidance and support has allowed for the completion of this work. I would like to acknowledge Dr. Oludamilola Daramola who came in and exceptionally guided the SEAM Lab during Dr. Lee’s absence. Chad Able, Hamed Bateni, and Greg Horne provided guidance, knowledge, and friendship throughout my time at the SEAM Lab, even after they left to pursue other opportunities and for that I am extremely grateful. I would like to thank all of my professors that I have had throughout the years as they provided me with the knowledge needed to become the researcher that I am today. To all of my friends, whether we’ve been friends for many years or for a short period of time, you have been with me throughout this journey and have made my time in my undergraduate and graduate studies enjoyable and for that I thank you. Last but certainly not least, I would like to thank everyone who has worked at the SEAM Lab past and present, from undergraduate students to graduate students. You have all provided help at times and for that I am extremely grateful. 6 TABLE OF CONTENTS Page Abstract ............................................................................................................................... 3 Dedication ........................................................................................................................... 4 Acknowledgments............................................................................................................... 5 List of Tables ...................................................................................................................... 8 List of Figures ..................................................................................................................... 9 Chapter 1: Introduction ..................................................................................................... 12 Chapter 2: Literature Review ............................................................................................ 18 Chapter 3: Significance and Objectives ............................................................................ 21 Chapter 4: Experimental Methodology ............................................................................. 23 Section 1: Experimental Apparatus and Chemical Feedstocks .................................... 23 Section 2: Experimental Design ................................................................................... 27 Chapter 5: Results and Discussion .................................................................................... 32 Section 1: Acetic Acid .................................................................................................. 32 Section 2: Acetaldehyde ............................................................................................... 43 Section 3: Acetamide .................................................................................................... 49 Section 4: Connecting Trends ....................................................................................... 54 Chapter 6: Conclusions and Recommendations ............................................................... 57 References ......................................................................................................................... 60 Appendix A: Data Analysis Information .......................................................................... 63 A1: Density and Molecular Weight Data ..................................................................... 63 A2: List of Symbols ...................................................................................................... 63 A3: Acetamide Flowrate Calculation ........................................................................... 65 A4: Acetaldehyde Calculations .................................................................................... 66 7 A5: Acetic Acid Calculations ....................................................................................... 67 A6: Acetamide Calculations ......................................................................................... 68 A7: Error Calculations/Propagation .............................................................................. 69 Appendix B: Gas Chromatography Information............................................................... 73 B1: Gas Chromatography Instrument Method .............................................................. 73 B2: Calibration Curves ................................................................................................. 74 B3: Calibration Injections ............................................................................................. 77 Appendix C: Photos and Diagrams ................................................................................. 100 8 LIST OF TABLES Page Table 1: Test Matrix........................................................................................................27 Table 2: Schedule of experiments ...................................................................................29 Table 3: Acetic acid steady state effluent mole fractions ...............................................38 Table 4: Acetic acid effluent flow rate, hydrogen yield, gasification efficiency, carbon efficiency, and gasification rate ......................................................................................38 Table 5: Inconel 625 nominal composition ....................................................................40 Table 6: Haynes 282 nominal composition ....................................................................41 Table 7: Acetaldehyde steady state effluent mole fractions ...........................................47 Table 8: Acetaldehyde steady state effluent flow rate, hydrogen yield, gasification efficiency, carbon efficiency, and gasification rate ........................................................47 Table 9: Acetamide steady state effluent mole fractions ................................................53 Table 10: Acetamide steady state effluent flow rate, hydrogen yield, gasification efficiency, carbon efficiency, and gasification rate ........................................................53 Table A1: Density and molar mass of gases that constitute syngas ...............................63 Table A2: Density and molar mass of chemical feedstocks utilized ..............................63 Table A3: Slopes, intercepts, and their errors for the GC calibration curves .................69 Table B1: Standard gases used for calibration (Note: Gas 7 also had 15.1% butylene and 15.0% propylene and was only used to calibrate ethylene) ............................................78 9 LIST OF FIGURES Page Figure 1: Phase diagram for water ..................................................................................13 Figure 2: Density
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