Magnetocaloric materials can be useful in magnetic refrigeration applications, but to be practical the magneto-refrigerant needs to have a very large magnetocaloric effect (MCE) near room temperature for modest applied fields (<2 Tesla) with small hysteresis and magnetostriction, and should have a complete magnetic transition, be inexpensive, and environmentally friendly. One system that may fulfill these requirements is Mn x Fe 2-x P 1-y Ge y , where a combined first-order structural and magnetic transition occurs between the high temperature paramagnetic and low temperature ferromagnetic phase. We have used neutron diffraction, differential scanning calorimetry, and magnetization measurements to study the effects of Mn and Ge location in the structure on the ordered magnetic moment, MCE, and hysteresis for a series of compositions of the system near optimal doping. The diffraction results indicate that the Mn ions located on the 3f site enhance the desirable properties, while those located on the 3g sites are detrimental. The entropy changes measured directly by calorimetry can exceed 40 J/kg·K. The phase fraction that transforms, hysteresis of the transition, and entropy change can be controlled by both the compositional homogeneity and the particle size, and an annealing procedure has been developed that substantially improves the performance of all three properties of the material. On the basis of these results we have identified a pathway to optimize the MCE properties of this system for magnetic refrigeration applications.
In recent years, MnFePGe magnetocaloric materials have been widely studied as promising candidates for magnetic refrigeration materials. The Curie temperature of MnFePGe can be adjusted to around room temperature by changing the element ratio or doping with other elements. Due to its first-order magnetic and structural transition, it engenders a large entropy change but unfortunately also exhibits a large thermal hysteresis during the phase transition, which leads to energy loss and lower refrigeration capability. In this paper, we establish a correlation between the in-plane covalent bonding and Curie temperature (TC), thermal hysteresis (ΔThys), two-phase coexistence zone (ΔTcoex), and entropy change (ΔSDSC) using 54 Mn2−xFexPyGe1−yMz (where M is a metallic or nonmetallic doped element) samples with different components. Neutron diffraction and XRD diffraction data and refinements have been employed to allow a detailed electron density reconstruction of six typical samples with the maximum entropy method. We find that the length of the in-plane bonding is closely correlated with the TC and ΔThys, while the TC, ΔThys, ΔTcoex, and ΔSDSC have no significant correlation with the length of the interlayer covalent bond. Moreover, we find that the ΔThys correlates most strongly with the change in the bond length when undergoing the paramagnetic-to-ferromagnetic phase transition rather than the absolute value of the bond length. These results provide an understanding of how to control the properties, enabling effective ways to tune the composition of magnetic refrigeration materials to tailor magnetocaloric properties for optimal performance.
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