Significant reduction of phase-transition hysteresis for magnetocaloric (La1-xCex)2Fe11Si2Hy alloys by microstructural manipulation

Abstract

First-order magnetostructural phase transitions are inevitably accompanied by large hysteresis, which evokes non-ignorable energy losses a main challenge for the utilization of giant magnetocaloric effect (MCE) materials in the emerging magnetic cooling technology. In this work, we present a novel approach to reduce the hysteresis and simultaneously to remain the giant entropy change in La-Fe-Si-based MCE alloys by microstructural manipulation. The microstructure evolution is comprehensively studied by high angle annular dark field-scanning transmission electron microscope, three-dimensional atom probe and geometric phase analysis. For the LaFe13-xSix system via co-doping of Ce and H atoms, we have observed the appearance of nanograins in size range of 5 – 50 nm that is totally different from the widely reported compositions. Such refinement can be ascribed to the release of internal stress caused by the inhomogeneous distribution of hydrogen atoms. With the formation of the nanocrystals in (La1-xCex)2Fe11Si2Hy alloys, the value of hysteresis loss can be monotonously reduced from 48.3 to 0.6 J kg−1. More importantly, the magnetostructural transition keeps an obvious first-order type, which leads to a large adiabatic temperature change of 2.03 K in 1.3 T upon 105 magnetic cycles, as well as a high reversible refrigeration capacity of 89.4 J kg−1 for (La0.6Ce0.4)2Fe11Si2Hy.