Microfibrous Entrapped Catalysts for Low Temperature CO Oxidation

Abstract

AbstractLow temperature CO oxidation is characterized by slow reaction kinetics and CO self-poisoning of the catalyst, which compete with each other. A platinum catalyst with ceria as a promoter supported on a high surface area silica support has been developed. The catalyst has a significant activity for CO oxidation even in the presence of moisture. The catalyst showed a significant increase in activity with decreasing particle size (η<0.95, even at 100μm), indicating a clear transport limitation.In case of larger catalyst particles the diffusional resistances affect the reaction kinetics, leading to greater rates of CO self-poisoning causing deactivation of the catalysts. However, conventional packed bed of smaller particles poses problems such as high pressure drop, packing issues, bed channeling, flow maldistributions, and dead zones in the reactor bed, which result in poor inter-phase heat and mass transfer rates. Most of these problems are related to poor packaging of smaller particles, strongly suggesting the need for immobilization of small particles. A new class of micro-structured materials consisting of sorbents/catalysts entrapped in metal, ceramic, or polymer microfibers (MFES/MFEC) has been developed at Auburn University. These materials immobilize the small particles by sinter-locking them in fiber mesh. The immobilization of particles results in better heterogeneous contacting efficiency. Additional studies have shown that the high voidages and structural uniformity of the MFES lowered the flow maldistributions, eliminated the peaking flows between particles, and helped achieve better radial dispersion. Thus MFEC/MFES improved inter-phase transport rates.The Pt-CeO2/SiO2 catalyst entrapped in metal microfibers demonstrated a significant improvement in CO conversion compared to a conventional packed bed configuration while maintaining a lower pressure drop. Further catalyst entrapment in metal microfibers minimized cold spots in the reactor bed due to better intra-phase heat transfer rate. Higher effective thermal conductivity of MFEC improved the activity of the catalyst, which was particularly visible at high CO concentration wherein the CO inhibition kinetics takes over. For example, MFEC with 1/3 rd of catalyst loading as that of packed bed of same particle size, outperformed packed bed configuration.The catalysts were prepared by incipient wet impregnation. Surface characterization of catalysts was carried out using CO, H2, O2 chemisorption, O2 – H2 titration, N2 physisorption, powder XRD, and was correlated with catalytic activity.This microfibrous entrapped catalyst demonstrated a great potential for low temperature CO oxidation. These MFEC can be used in air purification, emergency escape products, and as a cathode air filter for PEM fuel cells.