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Chapter 5. Aspects of Metal-YSZ Electrode Kinetics 164 cermets. The first report from a study currently being carried out by Utz et al [22] on Ni pattern electrodes provides a good review of other pH2O dependencies found in literature, and is consistent with the above. The greater bias dependence with coarser microstructure might be related to the possible activation by accumulation of adsorbed intermediate species discussed in section 5.3.4.2 and section 5.3.4.3. The species would accumulate on either the metal surface, the YSZ surface, or both. Coarser structures have more surface per TPB than finer structures, providing more area for accumulation. The inductive loops observed in some impedance spectra measured under bias are consistent with adsorbed intermediates (sections 5.3.4.2 and 5.3.5.1). Based on the discussion above, it does not seem likely that the previously proposed [15] mobilization of impurities by their reaction with product H2O during anodic bias plays a major role in the bias dependence (or pH2O dependence), although that might also be occurring to some extent. Several mechanisms have been proposed for the pH2O dependence of the polarization resistance for Ni. One is that it can be simply explained by ―equilibrium-potential effects alone, without the necessity of assuming any additional kinetic or catalytic effect‖ [83]. In light of the results of the present study – increasing RP with higher pCO2 in CO/CO2 atmospheres for Ni, and an opposite response in H2/H2O (increasing RP with higher pH2O) for Pd versus Ni – this explanation seems unlikely. Another proposed mechanism is based on the higher pH2O leading to a hydroxylated YSZ surface which allows the migration of H+ on the YSZ [21]. Presumably this mechanism would be independent of the metal electrode material, however in the present study Pd exhibits the opposite pH2O dependency. That does not rule out the YSZ-hydroxyl mechanism for Ni, though, because the mechanism may be different for Pd. For Pd, the increase in pH2O might bring about a competing phenomena that is more detrimental to performance than any improvements the adsorbed hydroxyls on YSZ might bring. For example, the increase in pH2O might block adsorbed/absorbed hydrogen on Pd. There is no reason that the same adsorbed intermediates that might be accumulating during polarization are not also more available in higher pH2O. The magnitude of the capacitance is worth considering. For the impedance spectra shown in Figure 5-9 and Figure 5-10, the change from 3% H2O/H2 to 50% H2O/H2 results in a ~50% increase in the capacitance, which is calculated according to equation (5.3). (5.3) The capacitance changes from about 8 103 to 12 103 μF/cm2. This magnitude is characteristic of a chemical capacitance, not a double-layer capacitance. Adsorbed intermediate species are known to cause such a pseudo-capacitance. An increase in the capacitance could simply be due to the adsorption of more of the species that cause it. Compared with this 3%PDF Image | Electrolysis of CO2 and H2O
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