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Mn compounds presenting magneto-structural phase transitions are currently intensively studied for their giant magnetocaloric effect; nevertheless, several parameters remain to be further optimized. Here, we explore the Mn(Fe,Ni)(Si,Al) series, which presents two advantages. The Mn content is fixed to unity ensuring a large saturation magnetization, and it is based on non-critical Si and Al elements instead of the more commonly employed Ge. Structural and magnetic properties of MnFe0.6Ni0.4Si1-xAlx compounds are investigated using powder X-ray diffraction, SEM, EDX, DSC, and magnetic measurements. We demonstrate that a magneto-structural coupling leading to transformation from ferromagnetic with orthorhombic TiNiSi-type structure to a paramagnetic hexagonal Ni2In-type phase can be realized for 0.06 &lt; x ≤ 0.08. Unfortunately, the first-order transition is relatively broad and incomplete, likely as the result of insufficient sample homogeneity. A comparison between samples synthesized in different conditions (as-cast, quenched from 900 °C, or quenched from 1100 °C) reveals that Mn(Fe,Ni)(Si,Al) samples decompose into a Mn5Si3-type phase at intermediate temperatures, preventing the synthesis of high-quality samples by conventional methods such as arc-melting followed by solid-state reaction. By identifying promising MnFe0.6Ni0.4Si1-xAlx compositions, this study paves the way toward the realization of a giant magnetocaloric effect in these compounds using alternative synthesis techniques.

Drastic Influence of Synthesis Conditions on Structural, Magnetic, and Magnetocaloric Properties of Mn(Fe,Ni)(Si,Al) Compounds