Designing Electric Field Assisted Catalytic Reactors for Hydrogen Production Applications
Gray, Jake T.
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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. 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.