Tailored electrochemical properties by defect engineered pyrochlore structured samarium ruthenate
摘要
The structural and electrochemical properties of Sm2Ru2O7 synthesized with a minor Sm2O3 secondary phase has been investigated to understand the origin of mixed charge-storage mechanisms in supercapacitors. X-ray diffraction confirmed the coexistence of cubic Sm₂Ru₂O₇ and Sm₂O₃ with an average crystallite size of 28 nm and measurable lattice strain, indicating two different secondary-phase occupancy within lattice voids. Rietveld refinement revealed significant ion disorder and partial occupancies within the pyrochlore framework. The refined structural model is distributed over two correlated phases of strong Sm–O occupancy coupling. The refinement confirms the formation of defect-engineered lattice promoting both surface-controlled electric double-layer capacitance (EDLC) and fast reversible Faradaic reactions (pseudocapacitance) because of the oxygen-rich and oxygen-deficient site distributions. The active electrode exhibits a high specific capacitance of 451 F/g at 1 A /g in a three-electrode configuration, retaining 97% capacitance after 3000 cycles with a charge transfer resistance of 36 Ω. An asymmetric two-electrode device delivers 91 F/g at 1 A/g, an energy density of 18.2 Wh/kg, and 100% capacitance retention over 2500 cycles with reduced resistance (20 Ω). The coexistence of these mechanisms originates directly from crystallographic disorder, oxygen non-stoichiometry, and multiphase coupling enhancing the capacitive performance in two and three electrode supercapacitor devices.