OPERATION OF SOLID OXIDE FUEL CELL ANODES WITH PRACTICAL HYDROCARBON FUELS

摘要

This work was carried out to achieve a better understanding of how SOFC anodes work with real fuels. The motivation was to improve the fuel flexibility of SOFC anodes, thereby allowing simplification and cost reduction of SOFC power plants. The work was based on prior results indicating that Ni-YSZ anode-supported SOFCs can be operated directly on methane and natural gas, while SOFCs with novel anode compositions can work with higher hydrocarbons. While these results were promising, more work was clearly needed to establish the feasibility of these direct-hydrocarbon SOFCs. Basic information on hydrocarbon-anode reactions should be broadly useful because reformate fuel gas can contain residual hydrocarbons, especially methane. In the Phase I project, we have studied the reaction mechanisms of various hydrocarbons--including methane, natural gas, and higher hydrocarbons--on two kinds of Ni-containing anodes: conventional Ni-YSZ anodes and a novel ceramic-based anode composition that avoid problems with coking. The effect of sulfur impurities was also studied. The program was aimed both at achieving an understanding of the interactions between real fuels and SOFC anodes, and providing enough information to establish the feasibility of operating SOFC stacks directly on hydrocarbon fuels. A combination of techniques was used to provide insight into the hydrocarbon reactions at these anodes during SOFC operation. Differentially-pumped mass spectrometry was be used for product-gas analysis both with and without cell operation. Impedance spectroscopy was used in order to understand electrochemical rate-limiting steps. Open-circuit voltages measurements under a range of conditions was used to help determine anode electrochemical reactions. Life tests over a wide range of conditions were used to establish the conditions for stable operation of anode-supported SOFC stacks directly on methane. Redox cycling was carried out on ceramic-based anodes. Tests on sulfur tolerance of Ni-YSZ anodes were carried out.