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Chapter 6. Molybdate Based Ceramic Electrode Materials 173 very high performance. Some of the materials were found to have much higher performance in reducing H2O/CO2 than in oxidizing H2/CO, which is especially interesting for application as electrolysis electrodes. The results show that the high performance is attained sometimes by very different and unique mechanisms among different members of the materials families. SrTiO3, SrMoO3, and SrVO3 were found to form a solid solution. Without dopants, SrTiO3 is an insulator. On the other hand, SrMoO3 and doped variants have the highest electronic conductivity of all known oxides (higher than many metals), but are only phase stable in a narrow pO2 range, oxidizing to SrMoO4 and reducing to Mo and SrO. For the solid solutions, conductivity was gained from SrMoO3 and stability was gained from SrTiO3 and SrVO3. The electrochemical performance of these materials was high but not as high as that of the double perovskites. The double-perovskites were more stable than SrMoO3 and the solid solution. The double perovskite lattice allows Mo to be fully oxidized as Mo6+ (and therefore can be sintered in air) and tends to stabilize against strong reduction (but can still decompose if strong enough reducing conditions are applied). The double-perovskites, with 50 at% Mo on the B-site, had a lower conductivity than the solid solutions. Some of the double-perovskites exhibited much higher electrical conductivity than would be expected by the mechanism proposed for Sr2MgMoO6. Previously unreported phenomena were observed for the molybdates Sr2NiMoO6 and Sr2CoMoO6 which can explain the high electrical conductivity observed here as well as discrepancies in literature. At 800 °C in 9% H2/N2, Sr2NiMoO6 gradually decomposed to a multi-phase composite with enhanced electronic conductivity. Most notably, the decomposition resulted in the precipitation of nanoparticles of Ni and Mo-Ni alloy (and apparently other Sr-Mo-O phases) which lined the grain boundaries, forming chains. The surface of the decomposed materials was nanostructured and these nanoparticles were also present on all surfaces. Preparing a material and then performing controlled decomposition to form multiple desirable phases and a desirable microstructure (which can take place in situ) from these materials is considered as an interesting new way to prepare potentially high-performance electrode materials. The electrochemical activity of the decomposed Sr2NiMoO6 was very high for H2O/CO2 reduction and H2/CO oxidation, higher than any of the metal electrodes from Chapter 5 and comparable to the Ni metal electrode that had been activated by strong cathodic polarization. Sr2FeMoO6 did not decompose yet exhibited even slightly higher performance, due to a different mechanism most likely related to the defect chemistry of this material (possibly high mixed ionic-electronic conductivity) and/or the mixed valency of the Fe and Mo ions. The addition of Ti to the B-site, e.g. SrTi0.5Ni0.25Mo0.25O3, was found to prevent the decomposition. The polarization resistances of the best molybdate materials were two orders of magnitude lower than that of donor-doped strontium titanates. Many of the molybdate materials werePDF Image | Electrolysis of CO2 and H2O
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