Improving work temperature span and reversibility of magnetoelastic transition of (Mn,Fe)(2)(P,Si) alloys by Mg doping

Magnetocaloric materials with wide working temperature span and reversible magnetic transition are beneficial for the magnetic refrigerator. Besides of giant magnetocaloric effect, (Mn,Fe)(2)(P,Si) alloys exhibit significant thermal/magnetic hysteresis and a narrow working temperature span. In this work, the impact of Mg doping on the phase structure and magnetocaloric effect of Mn(1.05)Fe(0.9)P(0.5)Si(0.5-x)Mgx alloys has been studied. The results show that all samples crystallize into Fe2P-type main phase with little impurity phase. After Mg doping, the lattice parameter a of the main phase increases from 6.027(0) angstrom to 6.049(0) angstrom and c decreases from 3.488(6) angstrom to 3.480(6) angstrom, which leads to the increase of Curie temperature. Density functional theory calculation results confirm that the Mg atom located on the 2c site can increase the covalent bond length, and then enhance the ferromagnetic coupling between atoms leading to the increase of Curie temperature. Moreover, the first-order magnetic phase transition of Mn(1.05)Fe(0.9)P(0.5)Si(0.5-x)Mgx alloys is inhibited with the increase of Mg content, which results in the decrease of thermal/magnetic hysteresis and the increase of the effective working temperature span. For Mn1.05Fe0.9P0.5Si0.48Mg0.02 alloy, it has a Curie temperature of about room temperature, effective refrigeration capacity of 291.7 J center dot kg(-1), working temperature window of 46 K and magnetic entropy change of 9.4 J center dot kg(-1)center dot K-1. The alloy can be an excellent candidate in room temperature magnetic refrigeration devices with a wide temperature span.