Abstract
High potential to carbon deposition over metallic Fe0 greatly limits the improvement of methane-to-syngas selectivity via chemical looping technology. Herein, we found that the in-situ formed CeFexAl1−xO3 over ceria-hexaaluminate as “oxygen pool” could greatly improve carbon resistance even with presence of Fe0. Formation of CeFexAl1−xO3 only proceeds in ceria-hexaaluminate composite while not occurs in CeO2-Fe2O3-Al2O3, which was probably originated from the strong interaction between CeO2 and the adjacent Fe and Al ions in BaFe3Al9O19 hexaaluminate structure. CeFexAl1−xO3 with outstanding oxygen ion conduction capacity was in close contact with metallic Fe0 exsoluted from Fe-hexaaluminate in a unique CeFexAl1−xO3/Fe0/hexaaluminate sandwich-like structure, which provided a convenient pathway for CeFexAl1−xO3 as “oxygen pool” to supply sufficient oxygen for in-time oxidation of carbon over adjacent Fe0. Consequently, the recycled ceria-hexaaluminate displayed both outstanding carbon resistance and high CH4 conversion (∼90%) with enhanced syngas yield that 105% and 72% higher than CeO2-Fe2O3-Al2O3 oxide and Fe-hexaaluminate, respectively.
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