Effects of La-Co Co-Substitution and Magnetic Field Pressing on the Structural and Magnetic Properties of SrM Hexaferrites

We carefully investigated the effects of La-Co co-substitution and magnetic field pressing (MFP) on the structural and magnetic properties of SrM hexaferrites. Samples composed of Sr1−xLaxFe12−xCoxO19 were sintered at 1230 °C for 2 h in air with sintering additives composed of 0.7 wt% CaCO3 and 0.7 wt% SiO2. A single M-type phase was confirmed to exist up to x = 0.3. Rietveld refinement revealed a slight decrease in lattice parameter a and the unit cell volume (Vcell) with an increasing x, while parameter c showed a significant decrease. The saturation magnetization (Ms) values increased from 70.90 to 72.40 emu/g with an increasing x from 0.0 to 0.15 and then decreased to 71.38 emu/g with further increasing of x to 0.3, while the anisotropy field (Ha) increased from 17.7 to 25.9 kOe, leading to a continuous increase in the intrinsic coercivity (Hci), from 3.52 to 5.00 kOe, respectively. Using the MFP process, the c-axis of M-type hexaferrite grains could be effectively aligned to the applied field direction, which significantly affected the microstructures and, thus, magnetic properties of samples. Unlike non-MFP samples, exhibiting a significant increase in the average grain size (davg) but almost unaltered average thickness (tavg) with an increasing x from 0.0 to 0.3, MFP-processed samples exhibited almost unaltered davg values but a continuous decrease in tavg. Consequently, the variation in remanent flux density (Br) versus x followed that of Ms versus x and thus exhibited the highest Br of 4.05 kG for x = 0.15, leading to the highest maximum energy product {(BH)max} of 3.62 MGOe. With an increasing x from 0.0 to 0.3, the Hci values continuously increased from 3.14 to 3.84 kOe mainly due to a continuous increase in Ha, although they were significantly lowered in comparison with those of non-MFP samples because of a large increase in Br for a given composition x. A higher Mr/Ms ratio always resulted in a larger (BH)max in our samples regardless of x. A careful comparison of the microstructures and magnetic properties between MFP and non-MFP samples provided valuable insights into a broad area of permanent magnet optimization.