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Chapter 7. Conclusions and Outlook 218 resistance for co-electrolysis was slightly lower than for CO2 electrolysis and slightly higher than for H2O electrolysis, and closer to that of H2O electrolysis, suggesting that besides the CO2 and H2O electrolysis reactions, the reverse WGS reaction occurs. An impedance analysis technique, calculating the distribution function of relaxation times (DRT), was applied to identify the contributions of the various electrode processes to the total cell resistance. Comparison the DRTs of impedance measurements taken under systematically varied test conditions enabled clear visual identification of five electrode processes that contribute to the cell resistance. The processes could be assigned to each electrode and to gas concentration effects by examining their dependence on gas composition changes and temperature. A similar analysis had been done in prior work on different cells in different conditions. Here the technique was further applied to study the degradation mechanisms of the cell without relying on a model. The durability was tested at consecutively higher current densities (and corresponding overpotentials). By analyzing the impedance spectra before and after each segment, it was found that at low current density operation (–0.25 A/cm2 segment) degradation at the Ni/YSZ electrode was dominant, whereas at higher current densities (–0.5 A/cm2 and –1.0 A/cm2), the Ni/YSZ electrode continued to degrade but the serial resistance and degradation at the LSM/YSZ electrode began to also play a major role in the total loss in cell performance. This suggests different degradation mechanisms for high and low current density operation. Improving understanding of the reaction mechanisms at the negative-electrode that limit performance and cause it to deteriorate could enable significant improvements in the economics of the full system. In the point-contact metal electrodes study, widely different responses of the different metals to the same changes in test conditions (gas composition, temperature, and polarization) were observed, indicating that the same reaction mechanisms are not shared by the different metals, contrary to some recent studies. Evidence was also found that supports the explanation that impurities segregated to the TPB play a major role and are largely responsible for inconsistencies in the electrode kinetics literature. The significance of microstructure at the TPB was also revealed – the electrodes were activated by an order of magnitude when subjected to extreme conditions of oxidation-reduction and strong cathodic polarization, which induced the formation of a micro/nanostructured TPB. These results, along with an examination of trends in electrode kinetics literature, suggested possible reaction mechanisms for H2O/CO2 reduction as well as H2/CO oxidation. Ceramic materials offer potential improvements in several aspects of solid oxide cell affordability. In the ceramic materials study, novel high performance materials were obtained that can provide high electronic conductivity and electrocatalytic activity as part of a solid oxide cell negative-electrode. Unique phenomena were observed for some of the materials – they decomposed into multiple, beneficial phases whichPDF Image | Electrolysis of CO2 and H2O
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