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Anodes for solid oxide fuel cell (SOFC) systems operating in multiple fuel environments: Effects of microstructure and composition

Posted on:2008-06-21Degree:Ph.DType:Thesis
University:University of Ottawa (Canada)Candidate:Grgicak, CatherineFull Text:PDF
GTID:2442390005461966Subject:Chemistry
Abstract/Summary:
This work examined several cermet materials as possible anode materials for solid oxide fuel cell (SOFC) systems operating in multiple fuel environments. In particular, these materials consisted of two phase M-YSZ (M = Ni, Cu or Co, YSZ = yttria stabilized zirconia) cermets synthesized via the gel-precipitation method. Relations between synthesis conditions and cermet structure/performance dominated the first section of this work. SOFC anode performance was correlated back to original synthesis conditions, whereby dM/dYSZ was controlled via the production of a crystalline intermediate.;Electrochemical characterization of Ni- and Co-YSZ anodes in H2 and H2S/H2 fuels was performed and each arc observed in the impedance curves was ascribed to a specific process. The high- and mid-frequency arcs were related to transport and charge transfer processes respectively. Non-traditional relationships between inverse Tafel (Lefat) slopes and temperature were observed. This resulted in a change in charge transfer coefficients with respect to temperature. By evaluating this dependence, a charge transfer coefficient of 1.5 for hydrogen oxidation on Ni-, Co- and NiS-anodes was determined. CoS-anodes resulted in a charge transfer coefficient of 0.2.;NiS- and CoS-anodes were stable in sour gas environments and selective towards the electrochemical oxidation of H2 over H2S as suggested by open circuit voltage and mass spectrometry.;Cell performances of and CoS-anodes in sour gas environments were stable over a 6 day period and showed no signs of deterioration. However, H 2S was required in the fuel stream to maintain optimal performance of these anodes. Once H2S was removed, the CoS-anodes reverted to Co-YSZ. For CoS-based anodes, optimum cell performance was maintained at a H2S content >1v/v%.;Investigations of bimetallic NiCu- and NiCo-anodes were also performed. The addition of Cu to Ni-based anodes resulted in larger metal particle sizes and decreased anode activity for hydrogen oxidation. Small additions of Co to Ni-based anodes showed a marked improvement in hydrogen oxidation activity. The bimetallic anodes were also tested in H2S/CH4 mixtures and showed good activity for all anodes tested over a 15 hour period.
Keywords/Search Tags:Anodes, SOFC, Fuel, Cell, H2S, Environments, Charge transfer
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