a1 Thermodynamics and Sustainable Energy Lab, Department of Mechanical Engineering and Materials Science, Duke University 303 Hudson, Box 90300 Durham, NC 27708-0300, USA
In this study, a novel flow-based method is presented to place catalytic nanoparticles into a reactor by sol-gelation of a porous ceramic consisting of copper-based nanoparticles, silica sand, ceramic binder, and a gelation agent. This method allows for the placement of a liquid precursor containing the catalyst into the final reactor geometry without the need of impregnating or coating of a substrate with the catalytic material. The so generated foam-like porous ceramic shows properties highly appropriate for use as catalytic reactor material, e.g., reasonable pressure drop due to its porosity, high thermal and catalytic stability, and excellent catalytic behavior.
The catalytic activity of micro-reactors containing this foam-like ceramic is tested in terms of their ability to convert alcoholic biofuel (e.g. methanol) to a hydrogen-rich gas mixture with low concentrations of carbon monoxide (up to 75% hydrogen content and less than 0.2% CO, for the case of methanol). This gas mixture is subsequently used in a low-temperature fuel cell, converting the hydrogen directly to electricity. A low concentration of CO is crucial to avoid poisoning of the fuel cell catalyst. Since conventional Polymer Electrolyte Membrane (PEM) fuel cells require CO concentrations far below 100 ppm and since most methods to reduce the mole fraction of CO (such as Preferential Oxidation or PROX) have CO conversions of up to 99%, the alcohol fuel reformer has to achieve initial CO mole fractions significantly below 1%. The catalyst and the porous ceramic reactor of the present study can successfully fulfill this requirement.
The results of the present study confirm that product gas mixtures with up to 75% hydrogen content and less than 0.2% CO content can be achieved, which is an excellent result. The reactor temperature can be kept as low as 220°C while obtaining a methanol conversion of up to 70%. The used PROX catalyst showed selective CO conversion rates above 99.5% for temperatures between 80 and 100°C in presence of large molar fractions of H2O and CO2.
(Online publication February 07 2012)