Lanthanum-Strontium-Iron-Copper-Based Perovskite Oxide: Structure-Reactivity Relationships in Catalytic Hydroxylation of Anisole
摘要
Perovskite oxides are known as promising materials for various catalytic redox processes due to their structural flexibility and tunable electronic properties. In this study, the A-site of the SrFe1−xCuxO3−δ, perovskite lattice was systematically modified to investigate the influence of lanthanum substitution on catalytic performance. Three perovskite materials with the compositions of SrFe0.7Cu0.3O3−δ, La0.5Sr0.5Fe0.7Cu0.3O3−δ and LaFe0.7Cu0.3O3−δ, were synthesized by the combustion method using hexamine as fuel and subsequently evaluated for the catalytic hydroxylation of anisole. Powder XRD pattern indicated that LFC crystallized to form orthorhombic perovskite structure. The presence of Fe4+, Fe3+, Cu2+ and Cu1+ in the LFC sample was confirmed by XPS analysis. Oxygen-TPD showed peaks corresponding to O2 desorption from oxygen vacancies, and a high concentration of oxygen vacancies was observed in strontium-containing perovskite. The developed catalyst system showed similar catalytic activity, with anisole conversion of 64% and 63% guaiacol selectivity under optimal reaction conditions. The recyclability analysis revealed that the presence of La reduces the fouling and coke formation, thereby facilitating retention of catalytic activity over several cycles. The above fact is further confirmed by the TGA analysis of the spent catalyst. The SFC and LSFC catalysts showed strong interactions between oxygen vacancies and organic species, which are responsible for the deactivation. The LFC catalyst has fewer oxygen vacancies, and shows better structural stability, reactivity, and coke resistivity. These results highlight the role of A-site substitution in modulating catalytic behaviour, providing insights into the design of coke-resistant perovskite catalysts for biomass-derived components transformations.
Graphical Abstract