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Chapter 5. Aspects of Metal-YSZ Electrode Kinetics 117 literature [37]. The time scale was similar to that for Ni wire electrodes in the literature, for this temperature range [11, 37] and much faster than for lower temperature of 500 °C [14]. The Newman relation [40] (5.1) (where is the electrolyte conductivity) has been shown to approximate the contact radius for point-contact electrodes on solid electrolytes with dimensions on the same order of magnitude as those used in these testsii. The initial decrease in corresponds to an increase in the contact area, which results from the creep of the metal wires at high temperature. The contact area of the Cu wires (Figure 5-3a) grew more and for a longer time period than that of the Ni wires (Figure 5-3b). The higher creep rate of copper corresponds to the lower melting point of copper. The higher melting point metals Pt and Pd crept similarly to Ni, while the lower melting point metals Ag and Au crept similarly to Cu. Also shown in Figure 5-3 is the length-specific polarization resistance, LSRP, as it varies with the varying RS. The significance of LSRP is discussed in the next section. The metal wire electrodes also sometimes ―un-crept‖ when returning to lower temperatures, as can be seen in Figure 5-4. At 850 °C, decreased until the temperature was elevated to 1000 °C, at which point decreased further and then stabilized at 63 Ω. Upon returning to 850 °C, increased slightly and re-stabilized, indicating that the contact area shrunk slightly. Whereas Cu, Ni, Pd, and Pt showed a stable contact area at 700-1000 °C, Ag and Au did not at 700-900 °C (the lower maximum temperature due to the melting point of Ag). During a test with Ag and Au electrodes, at one point both showed a quick decrease in RS (increase in contact area). While the exact reasons and conditions for this were unclear, because of this instability, because Ag and Au had the highest polarization resistance, and because the purity of Ag and Au were unknown, these metals were not studied further. One possibility for the increase in contact area is migration of the metal on the YSZ surface, which might be the case at least for Au according to the SEM micrographs shown in Figure 5-5. In the literature, noble metals such as Pt, Pd, and Ag were observed to migrate on YSZ surfaces and form dendritic structures [41 , 42] (although in that study they were in oxidizing atmospheres). ii The Newman relation was derived for an aqueous cell and is valid when the distance between the working and reference electrodes is infinite (large). Newman supported this experimentally by positioning the reference electrode at different distances from the working electrode. Analogous formulas have been derived for heat conduction (pointed out by Newman) and electrical circuits.PDF Image | Electrolysis of CO2 and H2O
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