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Chapter 6. Molybdate Based Ceramic Electrode Materials 208 may be related to the defect chemistry of SFM. A higher concentration of oxygen vacancies may be present in the material. In catalysis, SFM was observed to provide high catalytic performance for CH4 oxidation and this high performance was attributed to a high concentration of oxygen vacancies [111]. As discussed earlier, oxygen vacancies form in reduced SMM as a result of some of the Mo6+ ions accepting an electron and becoming Mo5+. In SFM, the Fe ions most likely are mixed-valent as well (Fe2+/3+), which might allow for yet more oxygen vacancies in the crystal lattice. The LSRP values can be compared with those measured on the metal point electrodes in Chapter 5. The best molybdate electrodes have significantly higher performance than any of the metals. Only by subjecting the metals to extreme conditions of oxidation or strong cathodic polarization, both of which enhanced the performance, could the performance of the metals approach that of these molybdates. However, for the metals, how long the enhanced performance will last, and to what degree the treatments can be used on porous electrodes, is unclear. Finally, the non-molybdate STN-CGO electrode exhibited interesting characteristics that are relevant to the discussions above regarding activity for CO/CO2 versus H2/H2O reactions and regarding cathodic activation. Figure 6-32a shows impedance spectra measured at OCV. As with the molybdates, the performance in 3% H2O/H2 was higher than in 50% H2O/H2. In this case, however, the performance was significantly higher – the LSRP was about a factor of 8 lower. Remarkably, this electrode showed higher performance in CO/CO2 than in H2/H2O – the LSRP was more than a factor of 2.5 lower in 50% CO2/CO than in 50% H2O/H2. Potential sweeps were also measured in the same gas atmospheres (Figure 6-32b). As with many of the molybdates, this electrode activates under cathodic polarization in H2/H2O atmospheres. However, in CO/CO2, the activation is only minor and the polarization curve for both anodic and cathodic directions is nearly linear, which means that either the cathodic activation phenomena is linked to H2/H2O or for this specific electrode composition a different reaction mechanism takes over in CO/CO2. For an STN electrode without the CGO particles, the shape of the potential sweep in CO/CO2 was the same as in H2/H2O, suggesting that CGO is a good catalyst for CO oxidation and CO2 reduction. The relatively higher performance in 50% CO2/CO than in 50% H2O/H2 holds for the entire range of overpotentials from –300 to +300 mV. The difference in performance becomes much larger in the anodic regime and much smaller at higher cathodic overpotentials due to the different shapes of the sweeps in 50% CO2/CO and 50% H2O/H2. Note that the measurements are not normalized to the TPB nor the contact area. This is because it was observed in the SEM after the test that the CGO particles spread out on the YSZ surface and on the electrode tip; the interface was not well-defined. Still, a rough estimate could be made which indicated that the polarization resistance was 1-2 orders of magnitude lower for the CGO-coated STN electrode than for an STN electrode without CGO, in bothPDF Image | Electrolysis of CO2 and H2O
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