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Designing Electric Field Assisted Catalytic Reactors for Hydrogen

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Designing Electric Field Assisted Catalytic Reactors for Hydrogen DESIGNING ELECTRIC FIELD ASSISTED CATALYTIC REACTORS FOR HYDROGEN PRODUCTION APPLICATIONS By JAKE T. GRAY A dissertation submitted in partial fulfillment of the requirements for the degree of DOCTOR OF PHILOSOPHY WASHINGTON STATE UNIVERSITY The Gene and Linda Voiland School of Chemical Engineering and Bioengineering DECEMBER 2019 © Copyright by JAKE T. GRAY, 2019 All Rights Reserved © Copyright by JAKE T. GRAY, 2019 All Rights Reserved To the Faculty of Washington State University: The members of the Committee appointed to examine the dissertation of JAKE T. GRAY find it satisfactory and recommend that it be accepted. Su Ha, Ph.D., Chair Norbert Kruse, Ph.D. Jean-Sabin McEwen, Ph.D. M. Grant Norton, Ph.D. ii ACKNOWLEDGMENT This dissertation would not have been possible without the assistance of a great many people—far too numerous to name, and many of whom I do not know. Let the rudimentary list that follows suffice, and accept my sincerest apologies for anyone inadvertently overlooked. I first gratefully acknowledge my funding sources, without whom this research would only have been an idea. Most of the work presented in this dissertation had its beginnings in my project as an undergraduate, which was financed in part by the DeVlieg Foundation and many of the supplies and equipment used throughout this dissertation were obtained through their generosity. The National Science Foundation Graduate Research Fellowship Program (NSF-GRFP Award #1347973) contributed to most of the rest of this work by directly supporting me as a researcher. Without this aid, I would not have been able to focus on research. Additional funding from the Korea Institute of Energy Research and from the U.S. Office of Naval Research helped to purchase more supplies and equipment as the research progressed and allowed the project to expand through collaboration with the Navy Undersea Research Program. The intellectual input of my committee drove this research forward: I thank Drs. Su Ha, Norbert Kruse, Jean-Sabin McEwen, and Grant Norton for their academic assistance, advice, and general support. I’d like to extend additional gratitude to Drs. Ha and Norton for their assistance in preparing my NSF-GRFP and Graduate Research Internship Program (GRIP) application packages. I gratefully acknowledge the involvement of numerous collaborators over the years: Dr. Fanglin Che for her detailed and insightful density functional theory support which was the progenitor of much of my work, and supplemented much of the rest; Kriti Agarwal for her iii assistance with the electrical engineering aspects of this research and COMSOL modeling work; Dr. John Izzo for his support and guidance while working at the Naval Underseas Warfare Center which helped to expand the project in new directions; and to the undergraduate students who worked closely with me to adapt new materials for this application: Matt Sundheim and Derek Burnett. Without our lab and office facilities and equipment and the people responsible for holding it all together, none of this research would have been possible. Although I am immensely grateful to the entirety of the WSU faculty and staff for their role in maintaining our facilities, I would like to recognize certain people specifically: Jim Pogue, Jennifer Starks, and Nicole Leavitt for always putting up with my complicated schemes, ordering my equipment and supplies, and recovering my travel expenses; Jo Ann McCabe for helping navigate the twisted labyrinth that is university finances; Burton “Billy” Schmuck for looking out for our safety and the safety of the community; Kate Konen for her patient help with all things technological (even if it was usually just a button we forgot to press); Samantha Bailey for taking care of the crucial behind-the-scenes bureaucratic headaches of graduate school; and to Valerie Lynch-Holm and Daniel Mullendore at the Francesci Microscopy and Imaging Center for training, advice, and keeping the microscopes in excellent condition despite the hordes of inconsiderate graduate students always fiddling with them. To my group members, past and present, I thank you for companionship both inside and outside the lab. Thanks for making graduate school slightly more tolerable: Xiaoxue “Christy” Hou, Shuozhen Hu, Tsai Garcia-Perez, Bita Khorasani, Parissa Ziaei, Qusay Bkour, Kaytee Villafranca, Xianghui “John” Zhang, Kai Zhao, Oscar Marin-Flores, Martinus “Martin” Dewa, iv Wei-Jyun “Will” Wang, Yilin Liu, and Mohamed “Mo” Elharati. I wish you all success and happiness wherever your paths may lead. To my friends outside the lab, thanks for helping keep me grounded and limiting the amount of time I spend thinking about research. I especially thank Justin Jurgerson for being an entertaining conversationalist, formidable board game adversary, and delightful dinner guest. For my family I am eternally grateful. You have supported me since childhood and I wouldn’t be half the man I am today without you. My mother, Corrina Gray; brother Aric Gray (and his wonderful wife, Jackie Gray); sister Caitlin Gray; and all of my grandparents: Sam and Debbie Duncan and Kent and Susan Gray. Although they are no longer here to appreciate it, I also acknowledge the family I lost during my graduate journey: my great-grandmother Edith Curtis; my grandmother Carolyn Pray; and my father, Loren Travis Gray. Despite my best efforts to drown myself in my work, you have always reminded me of what is most important in life. Finally, I thank my partner-in-crime, Julian Reyes. Your smile always brightens my day whether we’re getting lost in the mountains or getting fat together on the couch. v DESIGNING ELECTRIC FIELD ASSISTED CATALYTIC REACTORS FOR HYDROGEN PRODUCTION APPLICATIONS Abstract by Jake T. Gray, Ph.D. Washington State University December 2019 Chair: Su Ha Fundamental studies on the effects of strong electric fields (on the order of 1-10 V/nm) have been conducted in various forms for nearly a century. These investigations have revealed a surprising amount about the natural world: the presence of strong intrinsic electric fields is, in part, responsible for the high catalytic activity of many natural systems. Examples include catalysts ranging from enzymes for biochemical processes to zeolites in industrial-scale petroleum refining to frustrated Lewis acid-base pairs in specialized synthetic chemistry. With Nature as our inspiration, attempts at artificially recreating these highly reactive conditions have been ongoing (albeit sporadically) since at least the 1970s. Until recently, these experiments have been necessarily conducted in high-vacuum systems to avoid the dielectric breakdown associated with long-range high-intensity fields. A handful of attempts at high-pressure, high-throughput applications of this phenomenon have been attempted—but aside from a few promising observations, little progress has been made. vi Herein are presented recent contributions to this body of work focusing on the development of (i) new high-pressure, high-throughput, and high-field reactors for hydrogen-producing reactions and (ii) tools for future reaction engineers seeking to incorporate applied electric fields into their designs. To this end, Chapters 1 and 2 supply comprehensive foundational knowledge including the fundamental physics of electric field assisted catalysis as well as previous attempts at reactor or test apparatus design. Chapter 3 explores the mechanism for the hydrogen producing reaction of formic acid decomposition. This well-characterized reaction is then applied in Chapter 4 as a reactive probe to directly measure the applied field strength at catalyst active sites. A technique is also presented for visualizing the field structures generated across the catalyst. Chapters 5 and 6 delve deeper into more traditional hydrogen producing reactions via hydrocarbon steam reforming: methane in Chapter 5 and gasoline, diesel, and jet fuel surrogates in Chapter 6. Two reactor designs are investigated in detail throughout this dissertation: the integrated circuit reactor in Chapters 4 and 5 and the coaxial capacitor reactor in Chapter 6. Suggested next steps for future researchers are provided in Chapter 7. vii TABLE OF CONTENTS Page ACKNOWLEDGEMENT ............................................................................................................. iii ABSTRACT ................................................................................................................................... vi LIST OF TABLES ......................................................................................................................... xi LIST OF FIGURES ...................................................................................................................... xii PREFACE ........................................................................................................................................1 CHAPTER 1: INTRODUCTION ....................................................................................................3 Section 1.1. Transport .............................................................................................................3 Section 1.2. Molecular Orientation .........................................................................................7 Section 1.3. Electronic Structure ..........................................................................................10 Section 1.4. Kinetic and Thermodynamic Changes ..............................................................16 Section 1.5. Intrinsic
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