Doctor of Philosophy (PhD)
Materials Science and Engineering
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SOFC, IT-SOFC, proton conducting, anode, cathode, H2S, CO2
Date of Defense
Proton conducting intermediate temperature (600oC-400oC) solid oxide fuel cells (IT-SOFC) have many potential advantages for clean and efficient power generation from readily available hydrocarbon fuels. However, it still has many unsolved problems, especially on the anode where the fuel got oxidized and the cathode where oxygen got reduced. In this study, for the anode, the effects of hydrogen sulfite (H2S) and carbon dioxide (CO2) as fuel contaminants were studied on the nickel (Ni) based cermet anode of proton conducting IT-SOFC using proton conducting electrolyte of BaZr0.1Ce0.7Y0.1Yb0.1O3 (BZCYYb). Both low-ppm level H2S and low-percentage level CO2 caused similar poisoning effects on the anode reaction. The H2S poisoning effect was also found to be much less than on oxide-ion conducting SOFC, which is attributed to the absence of water evolution for the anode reaction in proton conducting SOFC. In addition, the H2S/CO2 poisoning mechanisms were investigated using X-ray diffraction, energy dispersive spectroscopy (EDS), Raman spectroscopy, and secondary ion mass spectroscopy (SIMS). For H2S, other than possible sulfur dissolution into BZCYYb, no bulk reaction was found, suggesting sulfur adsorption contributes to the reduced performance. For CO2, reaction with BZCYYb to form BaCO3 and CeO2 is identified and is believed to be the reason for the sudden worsening in CO2 poisoning as temperature drops below ~550oC. For the cathode, several representative SOFC cathodes including silver (Ag), La0.6Sr0.4Co0.2Fe0.8O3-δ (LSCF), LSCF-BZCYYb composite, and Ba0.5Sr0.5Co0.8Fe0.2O3-δ (BSCF) were evaluated based on BZCYYb electrolyte. LSCF give similar high interfacial resistance as Ag, while LSCF-BZCYYb composite cathode shows lower interfacial resistance, suggesting LSCF behaves like pure electronic conductor cathode in this case. For BSCF, it shows smallest interfacial resistance and the charge transfer process appears to accelerate with the introduction of H2O, while oxygen adsorption/transport seem to slow down due to adsorbed H2O. Furthermore, CO2 was shown to cause poisoning on the BSCF cathode, yet the poisoning was significantly reduced with the co-presence of water. The results suggest that although BSCF seem to display mixed proton-electronic conduction, its strong affinity to H2O may inhibit the oxygen reduction reaction on the cathode and new cathode materials still need to be designed.
Sun, Shichen, "Electrochemical Behaviors of the Electrodes for Proton Conducting Intermediate Temperature Solid Oxide Fuel Cells (IT-SOFC)" (2018). FIU Electronic Theses and Dissertations. 3915.
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