Liquid-solid phase separation of permalloy in liquid Mg results in selectively dissolved Ni, which provides a unique opportunity for the design of immiscible heterogeneous composite materials and the comprehensive metal recycling of permalloy scraps. A guideline of the alloy design for the liquid-solid phase separation system was proposed. The effects of immersion temperature and time on the Ni extraction were studied by an experimental method. The diffusion behavior of Ni from the permalloy to liquid Mg and the microstructure evolution in the permalloy during the liquid-solid phase separation were discussed. The results show that the Ni in the permalloy was quickly extracted into the liquid Mg and formed an Mg-Ni alloy, while the other components such as Fe, Co, and Mn were held back in the phase-separated permalloy. The phase-separated permalloy with the solidified Mg exhibits a three-dimensional (3D) Fe/Mg bicontinuous composite structure. Furthermore, simple treatments were carried out for the reaction products such as the Fe/Mg bicontinuous composite and the Mg-Ni alloy, and the recycling strategies for functionalization of these treated reaction products were provided. A 3D porous Fe-based alloy with electromagnetic interference (EMI) shielding efficiency of 52 dB can be obtained if Mg is removed from the Fe/Mg bicontinuous composite. Instead of the complete separation of pure Ni from the recycled Mg-Ni alloy by vacuum distilling, the Mg-Ni alloy can be enriched into Mg2Ni as an initial hydrogen storage material.
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