Perovskite-type oxides show irrefutable potential for feasible thermochemical solar-driven CO2 conversion. These materials exhibit the exact characteristics required by the low temperature reverse water-gas shift chemical looping process. These properties include structural endurance and high oxygen redox capacity, which results in the formation of numerous oxygen vacancies, or active sites for CO2 conversion. A major drawback is the decrease in oxygen self-diffusion with increasing perovskite particle size. In this study, the La0.75Sr0.25FeO3 (LSF) perovskite oxide was combined with various supports including popular redox materials CeO2 and ZrO2 along with more abundant alternatives such as Al2O3, SiO2, and TiO2, in view of its potential application at industrial scale. Supporting LSF on SiO2 by 25% mass resulted in the largest increase of 150% in CO yields after reduction at 600 °C. This result was a repercussion of significantly reduced perovskite particle size confirmed by SEM/TEM imaging and Scherrer analyses of XRD patterns. Minor secondary phases were observed during the solid-state reactions at the interface of SiO2 and TiO2. Density functional theory-based calculations, coupled with experiments, revealed oxygen vacancy formation only on the perovskite phase at these low temperatures of 600 °C. The role of each metal oxide support towards suppressing or enhancing the CO2 conversion has been elucidated. Through utilization of SiO2, the reverse water-gas shift chemical looping process using perovskite-based composites was significantly improved.
| Identifer | oai:union.ndltd.org:USF/oai:scholarcommons.usf.edu:etd-8825 |
| Date | 12 March 2018 |
| Creators | Hare, Bryan J. |
| Publisher | Scholar Commons |
| Source Sets | University of South Flordia |
| Detected Language | English |
| Type | text |
| Format | application/pdf |
| Source | Graduate Theses and Dissertations |
| Rights | default |
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