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Chapter 5. Aspects of Metal-YSZ Electrode Kinetics 143 mV. In H2/H2O, Pt was activated by anodic polarization and mostly relaxed within about 10 hours, whereas cathodic polarization, which had a higher LSRP during measurement, did not cause any activation – but after the measurement it slowly activated. In CO/CO2, Pt was unaffected by anodic polarization but significantly activated by cathodic polarization, after which it did not fully relax even after 50 hours. The above observations are summarized in Table 5-4. For all of the different metals, there is generally a correlation between the degree of activation during the +300 mV or –300 mV measurement and the rate of relaxation, except for Cu where even strong activation during measurement is followed by almost immediate relaxation. The anodic activation of Ni coincides with the activation at high anodic overpotentials discussed in section 5.3.4.1 and evident in the hysteresis of the polarization curves. However, the seemingly more permanent anodic activation in CO/CO2 is not reflected in the polarization curves. It is also surprising that Pd is so strongly and more permanently activated by anodic bias in H2/H2O and by cathodic bias in CO/CO2 considering the lack of hysteresis in the corresponding polarization curves (Figure 5-16c). Activation is most likely the result of either accumulation of reactive species or changes in morphology (such as an increase in the TPBL). —Accumulated species. One possible explanation for the seemingly permanent activations and their apparent non-existence in the polarization curves is that abruptly stopping the polarization leaves the interface is a more activated state than when the overpotential is gradually reduced. Species might have accumulated and are left to accelerate the much slower OCV reactions for a long time, whereas when the potential is ramped down these species are consumed with less and less being added. These species could be: adsorbed intermediates on the metal or YSZ surface absorbed intermediates in the metal or YSZ bulk holes injected into the YSZ subsurface, as discussed in the prior section. However, as already discussed, this seems unlikely since a decrease in RS was not observed. The fact that the long-term activation was only present for some metals suggests that if accumulated species are responsible, they are present in or on the metal, not the YSZ. Whether they are adsorbed or adsorbed probably depends on the metal. The Pd–H system is well known – during H2 oxidation the Pd electrode might store a significant amount of hydrogen atoms. The activation of the Pd electrode after CO2 electrolysis seems to indicate that Pd and carbon oxides have some kind of affinity as well. Ni–C is also well known, in that Ni is a goodPDF Image | Electrolysis of CO2 and H2O
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