Contrasting shell thickness-dependent magnetic behaviors of CoFe2O4@Fe3O4 and Fe3O4@CoFe2O4 core/shell nanoparticles

The magnetic properties of bi-magnetic core/shell nanoparticles (NPs) have been a subject of extensive investigation. Yet, the role of shell thickness in hard/soft and soft/hard core/shell NPs, corresponding to conventional and inverse structures, remains incompletely elucidated. In this study, we synthesized two sets of core/shell NPs, namely Fe3O4@CoFe2O4 (IF@CF) and CoFe2O4@Fe3O4 (CF@IF), featuring a fixed core diameter of approximately 11 nm and varying shell thicknesses up to 5 nm. These NPs were synthesized via a seed-mediated particle growth approach. The formation of the core/shell configuration of typical NPs in both sets was directly verified through scanning transmission electron microscopy-energy dispersive X-ray spectroscopy (STEM-EDS) imaging. Notably, the saturation magnetization (MS) of IF@CF NPs exhibited a significant increase compared to that of the IF core across all shell thickness variations, whereas it remained largely unchanged for CF core and CF@IF NPs. Conversely, the coercivity (HC) showed an opposite trend in the two structures with increasing shell thickness. We observed the emergence of a transition from constricted to smooth hysteresis loops in the conventional structure when the shell thickness reached 5 nm. The systematic evolution of hysteresis loops with escalating shell thickness in both structures closely correlates with distinct magnetic reversal mechanisms, influenced significantly by interparticle interactions. Our study presents a pathway for modulating the magnetic properties of bi-magnetic core/shell NPs, thereby opening avenues for advanced applications in magnetic imaging, sensing, drug delivery, and magnetic hyperthermia.