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Chapter 5. Aspects of Metal-YSZ Electrode Kinetics 127 For the Ni electrodes at 1000 °C in 97% H2 + 3% H2O, 3 processes were evident (Figure 5-9a). The high-frequency arc 1 had n-values (for the constant phase element) close to unity (>0.97). For the mid-frequency arc 2, n was around 0.95. For the low-frequency arc 3, n was around 0.73. Sometimes a fourth small high-frequency arc was found (barely visible in the Bode plot in Figure 5-9a), which consistently contributed <2% to the total impedance. This can likely be ascribed to the porous Pt counter electrode: a symmetrical cell with this electrode painted on both sides of an 8YSZ pellet was tested and the magnitudes and the high summit frequency of the impedance response agrees well with this minor arc. All of the processes were found to be temperature-activated by approximately the same amount, and there was little to no change in shape of the IS with change in temperature. The shape of the IS in Figure 5-9a compares well with that found in literature for similar conditions with similar Ni wire electrodes contacting non-high-purity stabilized zirconia [11, 37, 43]. On the Ni electrode, it appears that an increase in pH2O causes a decrease in the impedance of the lower-frequency RQ elements, so much so that they become negligible and only one process remains (Figure 5-9b). The Cu electrode also needed 3 RQ elements for a low-error fit, and the impedance of these processes was also reduced with increasing pH2O (Figure 5-9c+d). One might consider that gas concentration effects can result in reduced RP with higher pH2O for solid oxide cells [46-48]. However, such contributions are expected to be negligible for point electrode tests [46, 47]. Furthermore, such processes should not be thermally activated, but for the measurements obtained here all three processes appear to have a strong and similar temperature dependence. Finally, the same effect was not seen with increased pCO2 in CO/CO2 atmospheres, and some of the point electrodes showed the opposite response in H2/H2O – both of these results are described below. This confirms that there are no gas concentration processes contributing to the IS. 5.3.3.2. Effects of Gas Composition The IS from the first set of gas variations – 3%, 20%, and 50% H2O with balance H2, and 20% and 50% CO2 with balance CO – at 1000 °C are shown in Figure 5-10. The fitted spectra for Ni shown in Figure 5-9 and discussed in the prior section are part of the variation shown in Figure 5-10c. The single-arc impedance observed at 50% H2O / H2 is further reduced by about 25% when continuing the variation to 62% H2O / H2 (not shown). The effects of the gas composition were further examined by gas variations with fixed pH2, fixed pH2O, fixed pO2 and fixed pCO2. The dependencies of LSRP on the partial pressure of a gas can be correlated by equation (5.1). This empirical correlation is discussed in references [1, 20, 49]. (5.1)PDF Image | Electrolysis of CO2 and H2O
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