Role of transition metal in perovskites for enhancing selectivity of methane to syngas

摘要

This work investigates the role of transition metal at the B-site of ABO(3)-type perovskite that affects the lattice oxygen transfer for the partial oxidation of methane. Two types, LaBO3 and La0.6Ca0.4BO3 (B = Fe, Mn, Co), were synthesized and investigated under repeated redox cycles. The Fe-based perovskite had a high tendency of partial oxidation, while the Co-based perovskite mainly led to the full oxidation of methane. The Co-based perovskite was enriched with the surface oxygen component due to the enhanced oxygen transfer from the lattice to the surface vacant site. On the other hand, the Fe-based perovskite showed a relatively low lattice oxygen transfer to the surface oxygen vacancy although it had the highest lattice oxygen ratio among the different B-site perovskites. The selectivity and the production amount of the syngas were improved when the amount of the surface oxygen was controlled by adjusting the re-oxidation extent of the carriers during the oxidation step. Through these experiments, La0.6Ca0.4FeO3, which showed the highest syngas productivity with utilizing earth-abundant metals, was selected as an optimal oxygen carrier for methane reforming. (C) 2018 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.