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Abstract: Hydrogen sulfide, usually considered to be an anode catalyst poison, strongly promotes methane oxidation over sulfur resistant catalysts. The role of H2S in oxidation of sour CH4 feed over a sulfur resistant SOFC anode catalyst at 850°C has been determined through thermodynamic and experimental studies. The anode material was an intimately mixed 50/50 mass ratio composite of La0.4Sr0.6TiO3−δ and YSZ. The power density improved dramatically from 2mWcm−2 with pure CH4 as fuel to more than 450mWcm−2 for CH4 containing 20% H2S. However, H2S was not the only fuel converted, and its interaction with CH4 was the key factor in enhancement of performance. The anode effluent gas mixture included H2S, SO2, H2 and CS2 consistent with thermodynamic predictions. The role of H2S in the CH4 oxidation mechanism was determined, and showed that CH4 and H2S must be considered together as a fuel and not as two separate fuels. The types of electrochemical reactions that occurred in the fuel cell were strongly dependent on potential. [Copyright &y& Elsevier]

Abstract: Whereas Ce0.9Sr0.1Cr0.5V0.5O3 is an active fuel cell anode catalyst for conversion of only the H2S content of 0.5% H2S–CH4 at 850°C, inclusion of 5wt% NiO to form a composite catalyst enabled concurrent electrochemical conversion of CH4. A fuel cell with a 0.3mm thick YSZ membrane and Ce0.9Sr0.1Cr0.5V0.5O3 as anode catalyst had a maximum power density of 85mWcm−2 in 0.5% H2S–CH4 at 850°C, arising only from the electro-oxidation of H2S. Using a same thick membrane, promotion of the anode with 5wt% NiO increased the total anode electro-oxidation activity to afford maximum power density of 100mWcm−2 in 0.5% H2S–CH4. The same membrane provided 30mWcm−2 in pure CH4, showing that the incremental improvement arose substantially from CH4 conversion. Performance of each anode was stable for over 12h at maximum power output. XPS and XRD analyses showed that an increase in conductivity of Ce0.9Sr0.1Cr0.5V0.5O3 in H2S-containing environments resulted from a change in composition and structure from the tetragonal oxide to monoclinic Ce0.9Sr0.1Cr0.5V0.5(O,S)3. [Copyright &y& Elsevier]

Abstract: The stability and activity in 0.5% H2S–CH4 of Ce0.9Sr0.1VO3 and Ce0.9Sr0.1VO4 anode materials for H2S-containing CH4 fueled SOFCs have been determined. XRD showed that Ce0.9Sr0.1VO4 was reduced when the fuel gas was 0.5% H2S–CH4, while Ce0.9Sr0.1VO3 remained stable over 24h at 950°C. Electrochemical tests in 0.5% H2S–CH4 showed stable performance at 950 and 800°C for cells comprising Ce0.9Sr0.1VO3|YSZ|Pt. Comparison of fuel cell performances using 0.5% H2S–CH4, 0.5% H2S–N2 and 5% H2S–N2 as feeds showed that Ce0.9Sr0.1VO3 was not active for oxidation of methane, but highly active for conversion of H2S. Electrochemical impedance results were consistent with the finding that the anode was activated only in an environment that contained H2S. Conductivity measurements showed there was an increase in conductivity in H2S-containing environments, and that this increase resulted from a change in composition and structure from the oxide to monoclinic Ce0.9Sr0.1V(O,S)3, as evidenced by XPS and XRD analyses. [Copyright &y& Elsevier]

Abstract: Undoped BaTiO3 perovskite oxide is more effective than SrTiO3 and La2Ti2O7 oxide as anode catalyst in SOFC fueled with H2S-containing methane. Electrochemical performance, impedance spectroscopy and other characterizations show that pure BaTiO3 is a good anode catalyst for conversion of methane in SOFC, especially in H2S-containing atmospheres. Compared with SrTiO3 and La2Ti2O7 samples, the BaTiO3−based fuel cell has higher resistance to carbon deposition, better electrochemical performance and much higher stability during long term operation. A maximum power density of 135 mW cm−2 was achieved at 900 °C with 0.5% H2S–CH4 in a fuel cell having a 300 μm thick YSZ electrolyte. High catalytic activity for methane conversion, mixed electronic and ionic conductivity, and the surface basicity of BaTiO3 unexpectedly provides promising performance as anodes in SOFC. [Copyright &y& Elsevier]

Abstract: The effects of H2S and H2O in the methane feed on carbon deposition in a La0.4Sr0.5Ba0.1TiO3 (LSBT) anode-based solid oxide fuel cell were investigated in this work under different operating conditions. Characterization was done using a combination of electrochemical, Fourier transform infra-red spectroscopy (FTIR), temperature-programmed oxidation (TPO) and X-ray photoelectron spectroscopy (XPS) measurements. As expected, carbon accumulation became more severe with increasing exposure time and operating temperature, but less severe in the presence of a current and/or steam. Addition of 0.5% H2S to the feed increased carbon accumulation and this carbon could not be removed effectively by co-feeding a small amount of steam to the anode. The resulting carbon was, however, easier to remove with oxygen as compared to that deposited by the H2S-containing dry feed. [Copyright &y& Elsevier]