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Chapter 3. Sustainable Hydrocarbon Fuels by Recycling CO2 with Renewable/Nuclear Energy 56 recombination just as in direct water thermolysis. The hydrolysis step also has difficulties, including the formation of a passivating layer, which reduces the reaction rate [69]. Similar two-step cycles aim to overcome these issues, favoring gas-solid separations and/or lower temperatures. The basic ferrite cycle (FeO/Fe3O4) enables gas-solid separations, but has proven to be impractical [24, 69, 70]. Recent investigations have focused on cycles using modified ferrites (substituted with Co, Ni, or Mn) or ceria based materials as the oxidation-reduction media for dissociation of H2O to yield H2 [24, 69, 71-76], CO2 to yield CO [24, 75, 77], or both to yield syngas [75, 78-81]. These materials can be reduced at a lower temperature (<1500 °C) and both the oxidized and the reduced phases remain solid, as with the basic ferrite cycle. Ceria and doped ceria are especially interesting materials in that they can release oxygen without a change in crystal structure, cycling between the oxidized oxygen- stoichiometric phase and the reduced oxygen-deficient phase [79]. Ceria-based materials might therefore be expected to retain their microstructure through the redox cycles. Although the microstructure may be redox-stable, the high temperature of the reduction step can lead to coarsening of the microstructure. Grain growth (and a corresponding loss of activity) was observed in porous ceria reduced at 1500 oC - but only during the first 100 cycles, whereafter the performance was stable for hundreds of cycles [79]. Despite the initial performance loss, the high long-term durability suggests that ceria-based materials are a promising thermochemical cycle redox medium. For ferrites and modified ferrites, which are more prone to sintering than ceria-based materials, supporting the material on or combining the material with zirconia or yttria-stabilized zirconia inhibits sintering and improves durability [23,71,74]. Sintering also might not be an issue for some materials. It appears that other ceria-based materials enable a much lower temperature cycle; Cr-doped ceria was recently reported to be significantly reduced at only 465 °C and re-oxidized at 65 °C [82]. Ceria is also a known catalyst for many reactions involving gasses containing carbon and hydrogen [75, 82]. Addition of Ni to Sm-doped ceria was found to catalyze direct formation of CH4 with high selectivity when using a low temperature oxidation step (400 °C) [79]. At other conditions, Ni was found to catalyze the deposition of carbon [79], which might be a desirable product in some cases. Ferrite cycles have also been studied for reduction of CO2 to carbon [78, 83-85]. Finally, it is worth noting that while ceria based materials offer a number of potential advantages, cerium oxides have high molecular weights, which can be a disadvantage since flows of heavy solids should be minimized. Similar materials have been tested in 3-step cycles with the involvement of hydroxide, MxOy MxOy-1 + 1⁄2 O2 (g) MxOy-1 + 2 NaOH Na2O·MxOy + H2 (g) Na2O·MxOy + H2O MxOy + 2 NaOH (g)PDF Image | Electrolysis of CO2 and H2O
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