Consistent c-axis orientation characteristics toward the direction of applied pressure of Y-type BaSrCo2Fe11AlO22 (BSCFAO-θ) were successfully prepared by the strategy of hot pressing. The samples’ magnetoelectric coupling performance was greatly enhanced by the strategy of hot pressing than that of the traditional solid reaction method. The magnetoelectric current of BSCFAO-θ (θ = 0°) (12.06 μA/m2) was nearly 5 times higher than BSCFAO-SS (2.24 μA/m2). The magnetoelectric polarization of BSCFAO-θ (θ = 0°) (32.82 μC/m2) was nearly 4 times higher than that of BSCFAO-SS (8.31 μC/m2). The magnetoelectric coupling coefficients of BSCFAO-θ (θ = 0°) (1880 ps/m) were nearly 4 times higher than those of BSCFAO-SS (404 ps/m). The enhancement of magnetoelectric polarization of BSCFAO-θ (θ = 0°) can be attributed to the uniform c-axis orientation, which reinforced magnetoelectric polarization compared with none orientation that eliminated the magnetoelectric polarization on grain boundaries. The magnetoelectric coupling performance of BSCFAO-θ presented a gradually decreasing trend with the angle changing from 0° to 90° for the changing of orientation. Compared with traditional solid reaction methods, the strategy of hot pressing inhibits grain growth and increases grain boundaries, thus facilitating the enhancement of grain boundaries’ resistivity, and the electrical resistivity of BSCFAO-θ (3.08 × 1010 Ω cm) was nearly 10 000 times higher than that of BSCFAO-SS (2.5 × 106 Ω cm), which also benefits the magnetoelectric polarization performance of BSCFAO-θ. Therefore, the hot-pressing strategy can contribute to the forming of oriented ceramics and enhance the grain boundaries’ resistivity to improve magnetoelectric coupling performance.
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