Enhanced ionic oxygen flow through mixed ionic-electronic conducting membranes: Directional dependence, composite construction and the partial oxidation of methane.

摘要

Mixed Ionic-Electronic Conducting (MIEC) membranes transport ions and electrons in a crystalline matrix. Ionic transport occurs through MIEC materials in the presence of an applied ionic potential gradient. MIEC membranes form a special class of ionic conductors with primary applications as membrane separators, sensors, and components in solid oxide fuel cells.; Current efforts focus on separation of oxygen from air for supply to high temperature reactions. One such reaction is the methane partial oxidation to synthesis gas (CO and H2). Certain MIEC membrane characteristics are required for a methane partial oxidation reactor: (1) the cost of the material must be economical on a tube cost per mol oxygen transported basis; (2) the membrane must be stable in steep oxygen partial pressure gradients and in the presence of reducing gases; (3) the membrane must be stable at temperatures exceeding 800°C without fracturing due to thermal stress.; Two mechanisms govern the transport of oxygen through MIEC membranes: surface exchange at the MIEC/gas surface and ionic transport through the MIEC bulk. Most MIEC membranes conduct oxygen with a mixed transport mechanism, i.e., both surface exchange and bulk diffusion affect the total transport. We investigate the relative importance of bulk diffusion versus surface exchange in MIEC tubular and disk membranes made of La0.5Sr0.5Fe 0.8Ga0.2O3-delta.; We propose a proof based on the currently accepted transport model for the directional dependence of ionic flow through a tubular MIEC. We qualitatively confirm directional dependence using a novel experimental system. Further, we propose a model for ionic flow in a composite membrane system consisting of a dense, tubular LSFG substrate with a thin, dense layer of SrCox Fe1-xO3-delta applied to the surface(s). Comparisons are made between the performance of the monolithic membrane tube and the layered composite membrane tube. A layered composite tubular membrane is constructed and tested for ionic flow performance in this work. We also collect data for ionic flow through a dense tubular membrane with a 5-10 A film of platinum sputtered onto the surface. In addition, we obtain data for ionic flow at pressures exceeding 3 atm.