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Chapter 5. Aspects of Metal-YSZ Electrode Kinetics 129 In CO/CO2, Cu is the metal with the anomalous impedance responses, having negligible pCO dependence (Figure 5-11c and Table 5-3). Since the LSRP of Cu significantly increased when changing both CO and CO2 – from 20% CO2/CO to 50% CO2/CO (Figure 5-10b) – it may be dependent on pCO2. The CO/CO2 behavior of Pt in Figure 5-10h is not evident in the fixed pCO2 gas variation (Figure 5-11c and Table 5-3), suggesting that Pt may be activated by higher pCO2 and not by lower pCO. 5.3.3.3. Effects of Temperature The temperature dependence of the electrode impedance also provides information about the electrode kinetics. Using the Arrhenius relation, the activation energy can be obtained by multiplying k in equation (5.2) with the ideal gas constant. (5.2) Figure 5-12 shows the results of the temperature variation from 750-1000 °C in 3% H2O/H2, 50% H2O/H2, and 50% CO2/CO, along with the linear regression of the results in equation (5.2). The impedance closely follows this relation. As mentioned earlier, the shape of the IS did not appreciably change at different temperatures – all of the processes contributing to the impedance appear to have similar temperature activation. The activation energy (EA) of LSRP was quite similar for all of the metals: In 3% H2O/H2, it was in the range 1.4-1.7 eVfor Ni, Pd, and Pt, while for Cu it was about 2.0 eV. In 50% H2O/H2, all were in the range 1.3-1.6 eV. In 50% CO2/CO, all were in the range 1.8-2.0 eV. The EA for RS was 0.85 eV for 850-1000 °C or 0.8-0.9 eV in the 750-1000 °C range (not shown), which corresponds well with literature for the oxide ion conductivity of YSZ [49]. The EA for Ni, 1.4 and 1.6 eV in 3% H2O/H2 and 50% H2O/H2 respectively, agrees well with most results for Ni point electrodes in literature [1, 6, 7] as well as some Ni pattern electrodes [24]. On the other hand, a Ni point electrode prepared on high-purity single-crystal stabilized zirconia had a much lower EA of 0.9 eV [14] albeit at a lower temperature range, 500- 750 °C, and many finer-structure (pattern, porous, and cermet) electrodes have a similarly low EA [21,25,26].BakeretalreportedanEA forPdof~1.2eVin5%H2 +5%H2O+90%N2 in the 600-800 °C range [6], which is not far from the 1.3 eV found here in 50% H2O/H2 (same H2/H2O ratio). However, that same study reported only 0.8 eV for Pt, and here it is 1.5 eV in 50% H2O/H2.PDF Image | Electrolysis of CO2 and H2O
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