Nanostructured quaternary Ni1-xCuxFe2-yCeyO4 complex system: Cerium content and copper substitution dependence of cation distribution and magnetic-electric properties in spinel ferrites

Abstract

Quaternary Ni1-xCuxFe2-yCeyO4 complex nano-ferrites system with different cerium content ratio and copper substitution degree were synthesized via co-precipitation wet chemical technique. The newly obtained nanoparticles, with general formula Ni1-xCuxFe2-yCeyO4 (where x = 0.0, 0.3, 0.6 and y = 0.00, 0.03, 0.05, 0.08 and 0.10) were heated up to 600 °C to stabilize the specific crystalline spinel structure. The limit of cerium content was quantitively determined to be around 0.08 and up to 0.10. Furthermore, the powders were pelletized in a 13 mm wide pellets and thermally treated at 950 °C. The thermal treatment affected even more the phases segregation process, as CeO2 was identified in the sample with lowest degree of cerium insertion – 0.03. Also, a difference in color and size of pelletized samples was noticed after the 950 °C thermal treatment. The Rietveld refinement, crystal structure confirmation, morphology magnetic and electrical properties of samples have been deeply studied. The cation distribution carried out from Rietveld refinement confirms the occupancy of (Fe3+) on tetrahedral sites and [Ni2+], [Cu2+], [Fe3+] and [Ce2+] on octahedral sites in the crystal lattice. Preliminary information regarding the cation distribution in spinel structures were suggested by FTIR spectral results, precisely in the 650-520 cm−1 region, as a consequence of peak shape and lack of shiftiness of MTd – O bond. Spherical-shaped quaternary nano-ferrites of 17–28 nm were determined from FE-SEM analysis and the samples composition was confirmed by EDX analysis. Hysteresis loops shows modifications in coercivity, magnetization and magnetic remanence with Ni2+ and Cu2+ ions doping in Ni1-xCuxFe2-yCeyO4 complex systems with typical ferrimagnetic behavior. Dielectric measurements were employed in order to determine the electrical permittivity, dielectric losses and conductivity values in a 10 Hz – 1 MHz frequency range.