Excellent Cryogenic Magnetocaloric Properties in Heavy Rare-earth Based HRENiGa2 (HRE = Dy, Ho, or Er) Compounds

RENiX2 compounds, where RE = rare-earth element and X = p-block element, have been highly regarded for cryogenic magnetocaloric applications. Depending on the elements, they can crystallize in CeNiSi2-type, NdNiGa2-type, or MgCuAl2-type crystal structures, showing different types of magnetic ordering and thus affect their magnetic properties. Regarding the magnetocaloric effect, MgCuAl2-type aluminides show larger values than those of the CeNiSi2-type silicides and the NdNiGa2-type gallides due to the favored ferromagnetic ground state. However, RENiGa2 gallides can crystallize in either NdNiGa2- or MgCuAl2-type structures depending on the RE element. In this work, we select heavy RE (HRE) elements for exploring the microstructure, magnetic ordering and magnetocaloric performance of HRENiGa2 (HRE = Dy, Ho or Er) gallides. They all crystallize in the desired MgCuAl2-type crystal structure which undergoes a second-order transition from ferro- to para-magnetic state with increasing temperature. The maximum isothermal entropy change (∣∆Sisomax∣) values are 6.2, 10.4, and 11.4 J kg−1 K−1 (0–5 T) for DyNiGa2, HoNiGa2, and ErNiGa2, respectively, which are comparable to many recently reported cryogenic magnetocaloric materials. Particularly, the excellent magnetocaloric properties of HoNiGa2 and ErNiGa2 compounds, including their composite, fall in the temperature range that enables them for the in-demand hydrogen liquefaction systems.