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Recovering Valuable Products from the Aqueous Streams of Fast Pyrolysis Patrick Hefmon Hall Iowa State University

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Recovering Valuable Products from the Aqueous Streams of Fast Pyrolysis Patrick Hefmon Hall Iowa State University Iowa State University Capstones, Theses and Graduate Theses and Dissertations Dissertations 2017 Recovering valuable products from the aqueous streams of fast pyrolysis Patrick Hefmon Hall Iowa State University Follow this and additional works at: https://lib.dr.iastate.edu/etd Part of the Chemistry Commons, and the Mechanical Engineering Commons Recommended Citation Hall, Patrick Hefmon, "Recovering valuable products from the aqueous streams of fast pyrolysis" (2017). Graduate Theses and Dissertations. 16141. https://lib.dr.iastate.edu/etd/16141 This Dissertation is brought to you for free and open access by the Iowa State University Capstones, Theses and Dissertations at Iowa State University Digital Repository. It has been accepted for inclusion in Graduate Theses and Dissertations by an authorized administrator of Iowa State University Digital Repository. For more information, please contact [email protected]. Recovering valuable products from the aqueous streams of fast pyrolysis by Patrick Hefmon Hall A dissertation submitted to the graduate faculty in partial fulfillment of the requirements for the degree of DOCTOR OF PHILOSOPHY Major: Biorenewable Resources and Technology Program of Study Committee: Robert C. Brown, Major Professor Jacqulyn Baughman Thomas Daniels Mark Mba-Wright Marjorie Rover The student author, whose presentation of the scholarship herein was approved by the program of study committee, is solely responsible for the content of this dissertation. The Graduate College will ensure this dissertation is globally accessible and will not permit alterations after a degree is conferred. Iowa State University Ames, Iowa 2017 Copyright © Patrick Hefmon Hall, 2017. All rights reserved. ii DEDICATION To my dearest wife, Katie. iii TABLE OF CONTENTS Page LIST OF FIGURES ................................................................................................... v LIST OF TABLES ..................................................................................................... viii NOMENCLATURE .................................................................................................. x ACKNOWLEDGMENTS ......................................................................................... xii ABSTRACT………………………………. .............................................................. xiii CHAPTER 1 INTRODUCTION .......................................................................... 1 Biomass Structure ................................................................................................ 3 Thermochemical Processing ................................................................................ 6 Acetic Acid ......................................................................................................... 11 Levoglucosan ....................................................................................................... 14 Research Goal ...................................................................................................... 17 Dissertation Organization .................................................................................... 18 References ......................................................................................................... 19 CHAPTER 2 LITERATURE REVIEW ............................................................... 25 Barriers for Purification and Upgrading of Acetic Acid and Levoglucosan ....... 25 Acetic Acid ......................................................................................................... 27 Levoglucosan ....................................................................................................... 40 Chromatography .................................................................................................. 46 Review Summary ................................................................................................. 49 References ......................................................................................................... 49 iv CHAPTER 3 PURIFICATION OF PYROLYTIC SUGAR FROM BIO-OIL FRACTIONS ...................................................... 62 Abstract ......................................................................................................... 62 Introduction ......................................................................................................... 63 Materials and Methods ........................................................................................ 66 Results and Discussion ....................................................................................... 71 Conclusion ......................................................................................................... 75 Acknowledgements ............................................................................................. 76 References ........................................................................................................ 76 Supporting Information ....................................................................................... 81 CHAPTER 4 CHARACTERIZATION AND SEPARATION OF ACETATE FROM THE AQUEOUS PHASE OF BIO-OIL ............................. 85 Abstract ......................................................................................................... 85 Introduction ......................................................................................................... 86 Theory ......................................................................................................... 90 Materials and Methods ........................................................................................ 92 Results and Discussion ....................................................................................... 97 Conclusion ........................................................................................................ 112 References ......................................................................................................... 113 Supporting Information ........................................................................................ 117 CHAPTER 5 ADSORPTION RATES AND CAPACITY OF DEBITTERING AND ANIONIC RESINS TO RECOVER ORGANICS FROM THE AQUEOUS STREAM OF FAST PYROLYSIS .................... 120 Abstract ......................................................................................................... 120 Introduction ......................................................................................................... 121 Resin Structure and Properties ............................................................................. 123 Theory ........................................................................................................ 125 Materials and Methods ......................................................................................... 134 Results and Discussion ....................................................................................... 137 Conclusion ........................................................................................................ 144 References ........................................................................................................ 145 Supporting Information ....................................................................................... 150 CHAPTER 6 SUMMARY AND CONCLUSIONS ............................................. 153 v LIST OF FIGURES Page Figure 1-1 Structure of cellulose illustrating the β 1-4 glycosidic bonds between glucose molecules. ............................................................... 3 Figure 1-2 Structure of xylan ............................................................................... 4 Figure 1-3 Structures of paracoumaryl alcohol, coniferyl alcohol, and sinapinyl alcohol from left to right; primary monomers which comprise the majority lignin’s structure ............................................ 5 Figure 1-4 Fragment of lignin’s proposed structure ............................................ 6 Figure 1-5 Current schematic of the Pyrolysis Demonstration Unit. .................. 10 Figure 1-6 Structure of acetic acid....................................................................... 11 Figure 1-7 Structure of levoglucosan .................................................................. 14 Figure 3-1 Condensed pyrolytic sugar syrup. Its consistency is similar to food-grade maple syrup that is reddish-orange in color. ................... 65 Figure 3-2 Pyrolytic sugar composition (wt. %) of the raw and cleaned sugar samples are listed on a dry basis. Unidentified hydrolysable sugars were determined by subtracting total water soluble sugars from total hydrolysable sugar results. Table S1 in the supporting information contains the numerical data. ........................................... 73 Figure 3-3 Quantified characterized contaminants by category found in raw pyrolytic sugar syrup and cleaned pyrolytic sugars. Table S2 in the supporting information specifies each category’s compounds for GC-FID. Gas Chromatography – Mass Spectrometry (GC-MS) qualitative data is listed in Table S3. ................................................. 74 Figure 4-1 Equilibria in extraction of acetic acid from an aqueous solution using fatty acids as the solvent........................................................... 91 Figure 4-2 Heptanoic acid extraction of SF5. The topmost layer is heptanoic acid with the extracted organic portion, the bottom layer is immiscible material, comprised primarily
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