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Electrolysis of CO2 and H2O

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Electrolysis of CO2 and H2O ( electrolysis-co2-and-h2o )

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Chapter 1. Introduction 3 level, and materials and microstructure development. The experimental studies make extensive use of electrochemical impedance spectroscopy in conjunction with systematic variation of test conditions to examine the electrochemical phenomena. Variation of the material composition itself within families of similar materials was an additional parameter which was used in the electrode level and materials studies, which aimed to gain better understanding of the materials and electrochemistry versus studying a single material alone. Chapter 4 presents an experimental study of the performance and durability of co- electrolysis of CO2 and H2O using a solid oxide electrolysis cell. The cell resistance is broken down into contributions of several processes in the electrodes and electrolyte using an impedance analysis technique that enables clear visual identification of the processes. The technique is used to determine which processes degrade during long-term durability testing at three different current densities. High initial performance was observed for co-electrolysis, but the negative-electrode, a composite of nickel and yttria-stabilized zirconia (YSZ), is often the major site of cell degradation, including in the co-electrolysis results presented here. Therefore, to try to better understand the reaction mechanisms at the negative-electrode that limit performance and durability, the experimental study presented in Chapter 5 was carried out. The electrode kinetics of CO2 and H2O electrolysis and CO and H2 oxidation at the metal-YSZ interface were studied using a simplified point-contact electrode geometry with a well-defined electrode-electrolyte (metal-YSZ) interface. The simple geometry is useful for isolating the electrochemical properties without the effects of the complex microstructure of technological porous electrodes. A parameter used, which is uncommon in most studies, was the variation of the metal material itself – by comparing the same reactions using different metals (Ag, Au, Cu, Ni, Pd, and Pt) under identical conditions, the similarities and differences of the electrochemical responses between the different metals revealed more information about the reactions than a single material would have. Possible reaction mechanisms, and a number of interesting phenomena that occur at the metal-YSZ interface, are discussed. In Chapter 6, the metal based electrode is abandoned in favor of studying alternative electrode materials composed entirely of ceramic oxides. Ceramics can provide high electronic conductivity and electrocatalytic activity like nickel based electrodes, and additionally some ceramic materials have greater stability, can provide enhanced electrocatalytic activity via mixed ionic-electronic conductivity and/or nanostructured surfaces, and can be cheaper to produce since much of the material is made of oxygen. Fundamental properties (phase, microstructure, and electrical conductivity in the high-temperature reducing conditions relevant for solid oxide cell negative electrodes) of families of molybdate and titanate based ceramic materials were characterized. Certain material compositions exhibited very interesting properties, providing a nanostructured surface with high electronic conductivity upon exposure to operating conditions (high temperature reducing atmosphere). These materials were tested as electrodes to determine their electrocatalytic activity for H2O/CO2 reduction and H2/CO oxidation. The decomposed materials, as well as other materials from related molybdate families, exhibited very high

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