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Chapter 5. Aspects of Metal-YSZ Electrode Kinetics 128 Results of the gas variations at 850 °C and the linear regression of equation (5.1) using the results are shown in Figure 5-11 and Table 5-3 respectively. The same gas variations (but a less complete set) were performed at 1000 °C and the trends were nearly the same, but with usually somewhat shallower slopes (m values). Some trends in the dependence of the impedance on the gas composition can be clearly seen. —All of the metals showed better performance in 50% H2O/H2 than in 50% CO2/CO, by a factor of 10-25 at this temperature (Figure 5-10). In the literature, for Ni similarly large differences have been sometimes reported for porous Ni-YSZ cermet electrodes [32, 33]. On the other hand, other results have shown only 25-50% higher resistance for oxidation/reduction of CO/CO2 versus H2/H2O for porous Ni-YSZ cermet based cells [34, 50-52] (and see Chapter 4). —One can distinguish the relative electrocatalytic performance of the metals in different atmospheres (Figure 5-10). For the different metals, the relative electrocatalytic activities clearly vary with gas composition. The gas partial pressure dependencies identified below further describe this effect. The relative performance is further examined in the following section in regards to temperature dependency, and in regards to polarization in section 5.3.4. —Trends in the shapes of the impedance spectra are also observed (Figure 5-10). In 3% H2O/H2, Ni and Pd have nearly identical shape, and Cu and Pt have a different, nearly identical shape. Ni and Pd also have significantly higher performance than Cu and Pt in 3% H2O/H2, which might be due to the large low-frequency process that defines the shape of the Cu and Pt IS (e.g. see Figure 5-9c for Cu). It is worth noting also that only Ni seems to approach a single semicircle shape at any conditions. —Different pH2O, pH2, and pCO2 dependencies are observed for the different metals (Figure 5-10, Figure 5-11 and Table 5-3). Notably, when shifting to higher pH2O, Cu, Ni and Pt are all activated (LSRP is reduced), whereas Pd has the opposite response. In CO/CO2 atmospheres on the other hand, it is Pt that shows a different response than the rest, being activated by increased pCO2 whereas Cu, Ni, and Pd all show higher impedance. The ―fixed‖ gas variations reveal more information about these trends: In H2/H2O atmospheres, Ni and Pt show similar responses, LSRP having minor or negligible pH2 dependency and strong pH2O dependency (Figure 5-11a and Table 5-3). The dependency of LSRP on pH2O for Ni, m = –0.63, is within the range found in literature, –0.35 to –0.87 (and most often close to –0.5), for simple-geometry Ni electrodes [4, 7, 21, 22, 24, 25]. The lack of pH2 dependency also agrees with most literature (same references). While the LSRP of Cu also shows a similar trend, it does have a pH2 dependency and it has a somewhat weaker pH2O dependency. Pd shows anomalous behavior, with inverse dependencies on pH2 and pH2O compared with the other metals. This can be attributed to the Pd-H system (discussed further in following sections).PDF Image | Electrolysis of CO2 and H2O
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