A.N. Tabish
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5 records found
1
In this study, with the motivation of elucidating the effect of H2S and HCl on solid oxide fuel cell anodes, nickel and ceria pattern anodes are prepared on yttrium-stabilized zirconia electrolyte, and the effect of H2S and HCl on their performance is tested using electrochemical impedance spectroscopy. However, it has been found that while H2S adversely impacts both nickel and ceria, the poisoning caused is reversible for nickel and only partially reversible for ceria. Poisoning kinetics are similar and fast for both materials, while recovery kinetics are slower for ceria than nickel. High sulfur coverage is the rate-limiting factor inferred from the elementary kinetic modeling. Unlike H2S, the presence of HCl appeared to be favorable for electrochemical oxidation as the polarization resistance of both pattern electrode cells decreased upon feeding HCl contaminated hydrogen gas. Similar behavior has not been reported previously, and the conclusion regarding underlying mechanisms requires further investigation.
Using the Nernst-Planck-Poisson model and a detailed reaction mechanism, we studied the hydrogen electrochemical oxidation on a ceria anode. Resistances caused by surface kinetics, and bulk transport of oxide-ion vacancies and electrons are computed individually to identify the dominant resistive process. The effect of operating conditions like temperature and gas-phase composition on the polarization resistance is evaluated and compared with the experimental data obtained by Electrochemical Impedance Spectroscopy (EIS). The rate-determining step is found to be the charge-transfer reaction in which hydrogen adsorbs at the surface oxide ions and forms hydroxyls along with the charge-transfer to adjacent cerium ions. Based on the rate-determining step, the exchange-current density is also calculated and validated with the experimental data.
Fuel flexibility of solid oxide fuel cells enables the use of low cost and practical fuels like syngas. Understanding of the oxidation kinetics with syngas is essential for proper selection of anode material and its design optimization. Using nickel and ceria pattern anodes, we study the electrochemical oxidation of syngas in both dry and wet environments. In dry environment, the polarization resistance of CO oxidation drops drastically with the addition of small amounts of hydrogen to CO gas stream. In wet environment (4 % moisture), the polarization resistance of CO is only slightly higher than syngas and hydrogen. Observation in the first case is related to the hydrogen preferential oxidation whereas latter is a combined effect of water gas shift reaction and preferential oxidation of hydrogen. Kinetic modeling is also carried out to understand hydrogen and CO co-oxidation. Simulation suggests that CO, besides hydrogen, may also electrochemically oxidize depending upon its concentration in the syngas. At higher concentration, CO electrochemical oxidation may be non-negligible especially in case of ceria anodes.