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Development of a novel ceramic microchannel reactor for methane steam reforming

Murphy, Danielle M.
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Abstract
Microchannel heat exchanger and reactor technology has recently gained interest as an innovative way to improve heat-exchanger efficiency, reduce size and weight, and utilize thermal management capabilities to improve conversion, yield, selectivity, and catalyst life. Among many other possible applications, this technology is suitable for advanced recuperated engines, oxy-fired combustion processes for oxygen separation, gas-cooled nuclear reactors, recuperative heat exchanger and reformer units for solid oxide fuel cell systems, and chemical processing. This work presents the design, fabrication, and performance of novel ceramic microchannel reactors in heat-exchanger and fuel-reforming applications. Although most microchannel devices are made of metal materials, ceramics offer an alternative which enables significantly higher operating temperatures, improved tolerance to harsh chemical environments, and improved adherence of ceramic-based catalyst washcoats. Significant cost savings in materials and manufacturing methods for high-volume manufacturing can also be achieved. High-temperature performance of the ceramic microchannel reactor is measured through non-reactive heat-exchanger experiments within a dedicated test stand. Heat-exchanger effectiveness of up to 88% is experimentally established. After coating catalyst material over half of the reactor layers, use of the ceramic microchannel reactor in methane fuel-processing applications is demonstrated. As a fuel reformer, the ceramic microchannel reactor achieves process intensification by combining heat-exchanger and catalytic-reactor functions to produce syngas. Gas hourly space velocities (GHSV) up to 50,000 hr-1 with methane conversion higher than 85% are achieved. A complete computational fluid dynamics (CFD) model, as well as a geometrically simplified hybrid CFD/chemical kinetics model, is used in conjunction with experimentation to examine heat transfer, fluid flow, and chemical kinetics within the ceramic microchannel structure. While significant syngas formation is demonstrated, further work is necessary to optimize the catalyst, expand experimental process windows, and explore alternative uses for ceramic microreactors.
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