期刊
ACS CATALYSIS
卷 9, 期 9, 页码 8373-8382出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.9b02730
关键词
CH4 conversion; chemical looping reforming; Fe-based OCs; garnet; oxygen vacancy formation energy
资金
- National Science Foundation of China (NSFC) [21406225, 21573232, 21676269, 21706254]
- Postdoctoral Science Foundation of China [2014M561261]
It is of great significance to improve the syngas selectivity of Fe-based oxygen carriers (OCs), because of their sufficient lattice oxygen, low cost, and environmental compatibility in chemical looping partial oxidation of CH4. In this work, it was found that the addition of Y could remarkably increase CO selectivity of Fe2O3/Al2O3 to 98% with a CH4 conversion of , similar to 90%. X-ray diffraction (XRD) and transmission electron microscopy (TEM) characterizations combined with Mossbauer spectroscopy illustrated that the incorporation of Y led to the Fe species gradually transferring from Fe2O3 into the garnet structure (Y3Fe2Al3O12), a newly formed phase, which was found to be highly active for syngas generation. Density functional theory (DFT) calculations demonstrated that such a high CO selectivity of confined Fe species in garnet originated from enhanced oxygen vacancy formation energy (E-ov), compared with Fe2O3, which resulted from the lattice oxygen shared by not only reducible Fe ions but also nonreducible Al and Y ones in a garnet structure. Therefore, our work provides a meaningful guidance of new materials screening for methane partial oxidation in the chemical looping process.
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