A method for reducing the sulfur content of electrodeposited bulk nanocrystalline Fe–Ni alloys was developed to improve the tensile ductility of the materials and prevent thermal embrittlement caused by the grain boundary segregation of sulfur. Bulk nanocrystalline Fe–Ni alloys were prepared using electrolytes that primarily consisted of iron sulfate and nickel sulfamate combined with manganese chloride (MnCl2). The addition of MnCl2 in the deposition bath did not produce any significant changes in the Ni content and grain sizes of the electrodeposited alloys. In contrast, the sulfur content in the materials decreased from 840 to 620atppm. The bulk nanocrystalline Fe–Ni alloys with low sulfur content exhibited a higher tensile elongation of 16–19% compared to the materials with high sulfur content. Furthermore, after annealing at 200°C for 3h, The bulk nanocrystalline Fe–Ni alloys with low sulfur content exhibited a high tensile elongation of 9–10%, whereas the elongation of the materials with high sulfur content was 3%. The results indicate that the plastic elongation of electrodeposited bulk nanocrystalline Fe–Ni alloys can be improved by reducing the amount of sulfur in the materials.
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