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Novel ceramic materials based on molybdates with varying Mo valence were synthesized as possible alternative negative-electrode materials. The phase, stability, microstructure and electrical conductivity were characterized. The electrochemical activity for H2O/CO2 reduction and H2/CO oxidation was studied using simplified geometry electrodes, similar to the metals study. Unique phenomena were observed for some of the molybdate materials – they decomposed into multiple phases and formed a nanostructured surface upon exposure to operating conditions (in certain reducing atmospheres). The new phases and surface features enhanced the electronic conductivity and electrocatalytic activity. Preparing an electrode by performing controlled decomposition to form multiple desirable phases and a desirable microstructure (which can take place in situ) using these materials is a novel way to produce potentially high-performance electrodes for solid oxide cells. By modifying the composition, it was possible to prevent decomposition. Other members of the molybdate family exhibited similarly high electronic conductivity and electrocatalytic activity but did not decompose. The high activity was the result of a different mechanism, probably related to the defect chemistry of the material. 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 were significantly activated by cathodic polarization, and they exhibited higher performance for cathodic (electrolysis) polarization than anodic (fuel cell) polarization, which makes them especially interesting for use in electrolysis electrodes. Whereas nearly all of the molybdates showed higher performance for H2O electrolysis than CO2 electrolysis, one with vanadium showed nearly equal performance, and a non-molybdate which exhibits some complementary properties to the best molybdates, Gd-doped ceria in nanoparticle form, was found to be an excellent electrocatalyst for CO2 electrolysis and CO oxidation (moreso than for H2O/H2 for which it is known to be good).PDF Image | Electrolysis of CO2 and H2O
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