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The Production of Biobutanol from Biomass Via a Hybrid Biological/Chemical Process

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The Production of Biobutanol from Biomass Via a Hybrid Biological/Chemical Process University of Arkansas, Fayetteville ScholarWorks@UARK Theses and Dissertations 5-2015 The rP oduction of Biobutanol from Biomass Via a Hybrid Biological/Chemical Process Thomas Melvin Potts University of Arkansas, Fayetteville Follow this and additional works at: http://scholarworks.uark.edu/etd Part of the Algae Commons, Biochemical and Biomolecular Engineering Commons, and the Petroleum Engineering Commons Recommended Citation Potts, Thomas Melvin, "The rP oduction of Biobutanol from Biomass Via a Hybrid Biological/Chemical Process" (2015). Theses and Dissertations. 2050. http://scholarworks.uark.edu/etd/2050 This Dissertation is brought to you for free and open access by ScholarWorks@UARK. It has been accepted for inclusion in Theses and Dissertations by an authorized administrator of ScholarWorks@UARK. For more information, please contact [email protected], [email protected]. The Production of Biobutanol from Biomass Via a Hybrid Biological/Chemical Process The Production of Biobutanol from Biomass Via a Hybrid Biological/Chemical Process A dissertation submitted in partial fulfillment of the requirements for the degree of Doctor of Philosophy in Chemical Engineering by Thomas Potts Pittsburg State University Bachelor of Science in Physics, 1969 Pittsburg State University Master of Science in Physics, 1971 University of Arkansas Master of Science in Chemical Engineering, 2009 May 2015 University of Arkansas This dissertation is approved for recommendation to the Graduate Council. ___________________________________ Dr. Michael Ackerson Dissertation Director ____________________________________ ____________________________________ Dr. Robert Beitle Dr. Jamie Hestekin Committee Member Committee Member ____________________________________ ____________________________________ Dr. Christa Hestekin Dr. Mark Arnold Committee Member Committee Member Abstract Biobutanol use as a fuel began in the late 19th century. Problems remain in economic viability. A review of the state of the art and need for technical advances is presented. The technical potential of producing biofuel from a naturally occurring macroalgae was studied. The algae grow in Jamaica Bay, New York City, in contaminated water. The process consisted of mechanical harvesting, drying, grinding, and acid hydrolysis to form an algal sugar solution. Clostridium beijerinckii and C. saccharoperbutylacetonicum were used in an acetone butanol ethanol (ABE) fermentation to make butanol. Fermentation was followed by distillation Butanol concentrations during fermentation reached 4 g/L. The recovery of reducing sugars in the media was 0.29 g butanol/g sugar. Feedstock with greater than 7 g/L butyric acid caused death of the butanol-producing bacteria. The kinetics of the production of 1-octadecanol from octadecanoic acid was investigated in a liquid-phase trickle-bed reactor by hydrogenation. The primary reactions occurring in the reactor were the desired conversion of octadecanoic acid to 1-octadecanol and the subsequent undesired conversion of 1-octadecanol to octadecane. A series-parallel kinetics model first order in acid and zero order in hydrogen was developed to predict these two reactions. The activation energies of the reactions were 63.7.8 and 45.6 kJ/mole, respectively. The conversion of octadecanoic acid and the selectivity to the desired product as functions of temperature, space velocity, and inlet octadecanoic acid concentration were then estimated. The model predicts maximum productivity of 1-octadecanol at higher temperatures and short residence times. Parametric plots show productivity to be ≥0.48 g 1-octadecanol/g octadecanoic acid at 566 oF and a 0.1 h residence time. The model from the 1-octadecanoic acid study was fitted to several sets of data for the hydrogenation of butyric acid to butanol in the temperature regime of 300-400 oF and pressures of 700-1000 psig. The model failed to accurately predict the final concentrations of 1-butanol and butane. Reasons for this are suggested and future work to fix this problem is presented and discussed. Acknowledgments I would like to thank the Ralph E. Martin Department of Chemical Engineering for the opportunity to participate in this degree program. Special thanks go to Dr. Tom Spicer, Dr. Buddy Babcock, and Dr. Ed Clausen for their support, encouragement, and occasional prodding. My successful completion of the degree program would not have been possible without the efforts of those professors who served as research advisors. They provided guidance and challenging, interesting, and fun research projects on which to work. Serving as official advisers were Dr. Jerry King, Dr. Tom Spicer, Dr. Jamie Hestekin, Dr. Bob Beitle, and Dr. Mike Ackerson. Dr. Christa Hestekin served in this role in an unofficial capacity for two semesters, supervising a study of the pilot scale conversion of microalgae to 1-butanol and providing me funding and a major role in the study. Special thanks also go to my graduate research committee, who all played important roles in the progress of my research efforts. Dr. Mike Ackerson, Dr. Bob Beitle, Dr. Jamie Hestekin, Dr. Christa Hestekin, and Dr. Mark Arnold formed an awesome team and kept me on track throughout my studies. The department support personnel smoothed the path for me, and provided support and enthusiastic encouragement. George Fordyce, Harold Watson, and Jim Cole helped build much of the equipment necessary for my research. Amber Hutchinson and Jackie Schnippel helped keep my paperwork intact and helped every step of the way. Janet Lancaster deserves more thanks than can be expressed for the multitude of things she has done to keep me legal, honest, and at least partially under control. These people have become not only colleagues, but friends, and I will remember them always. All of my fellow graduate students have been great to work with, but certain of them have become close friends as well as fellow students. Dr. Jianjun Du and Dr. Keerthi Srinivas helped me get into the routine of being a student. Dr. Alice Jernigan worked with me on research, edited many of my papers, manuscripts, collaborated on classwork, fed me, offered a shoulder to cry on from time to time, and helped to keep me sane. She will be a friend for life. Dr. Lauren Merriman also edited my writing, collaborated with me on research, and became a life-long friend. Alex Lopez began his graduate school career as my mentee, but quickly became a collaborator, confidant, advisor, and friend. Dr. Ellen Brune and her husband Stuart have been enthusiastic cheerleaders and great support. Dr. McKinsie Fruchtl has been a collaborator, friend, and cheerleader. The University of Arkansas is a highly student-focused institution, and there have been several people in administrative roles that have gone out of their way to help me complete my scholastic journey. Dr. Collis Geren and Dr. Todd Shields provided me with encouragement and extra financial support. Dr. Patricia Koski and Dr. Susanne McCray offered encouragment, advice, and guidance. Finally, I would like to acknowledge the support and encouragement I recieved from my family, Dr. Melvin Potts, Doris Potts, Evangela Suzuki, Hiroshi Suzuki, Ian Suzuki, James Potts, and Judy Henderson. Table of Contents Chapter 1 Introduction ........................................................................................................ 1 Chapter 2 Biobutanol: An Important Biofuel And Bio-Product ..........................................5 Chapter 3 The Production of Butanol from Jamaica Bay Macro Algae ............................67 Chapter 4 Catalytic Production of 1-Octadecanol from Octadecanoic Acid Using Plug Flow Reactor Hydrotreating......................................................................95 Chapter 5 A Biological Fermentation of Biomass to Butyric Acid Followed by Catalytic Hydrogenation of the Butyric Acid to 1-Butanol .......................................112 Chapter 6 Conclusion .......................................................................................................140 Appendix 1 Matlab Code .................................................................................................153 List of Published Papers Chapter 2 – Published as a chapter in the book Applied Microbial Engineering Hestekin JA, Lopez AM, Clausen EC, Potts TM, Biobutanol: an important biofuel and bio- product. Appl Microb Eng 2013:450-87. doi:10.1201/b15250-18 Chapter 3 – Article Published in Environmental Progress and Sustainable Energy Potts T, Du J, Paul M, May P, Beitle R, Hestekin J. The production of butanol from Jamaica bay macro algae. Environ Prog Sustainable Energy 2012;31(1):29-36 Chapter 4 – Article Published in the Journal of the American Oil Chemist’s Society Potts TM, Durant K, Hestekin J, Beitle R, Ackerson M (2014) Catalytic Production of 1- Octadecanol from Octadecanoic Acid by Hydrotreating in a Plug Flow Reactor. J Am Oil Chem Soc 91: 1643-1650. DOI 10.1007/s11746-014-2501-7 Chapter 1 Introduction This dissertation has as its focus the production of fuel-grade 1-butanol from biomass waste products. The work began as a study of the fermentation of algal sugars obtained from the algae Ulva lactuca and expanded to the development of a broader methodology to produce 1- butanol from a variety of sugar solutions via a novel hybrid biological-chemical process. The first step of the hybrid process is the production of butyric acid from sugar solutions, and was not a part of this dissertation. The second step of this process is the liquid phase
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