Heterogeneous GdTbDyCoAl high-entropy alloy with distinctive magnetocaloric effect induced by hydrogenation

doi:10.1016/j.jmst.2021.08.076

Abstract

Abstract:

Developing novel magnetocaloric materials is of great significance for the applications of magnetic refrigeration. In this study, we designed a heterogeneous rare-earth-based high-entropy alloy (HEA) comprising amorphous matrix, local crystal-like cluster and nanocrystalline dihydride with average size of 7.5 nm through isothermal hydrogenation. This heterogeneous structure can significantly tune the magnetocaloric effect of alloy. After hydrogenation, the predominant exchange interaction transforms from ferromagnetic to antiferromagnetic with the disappearance of spin-glass-like behavior, and a complete second-order magnetic transition is obtained. Compared with the Gd₂₀Tb₁₈Dy₁₈Co₂₀Al₂₄ high-entropy metallic glass with a small number of nanocrystals, the maximum magnetic entropy change of the hydrogen-containing HEA is increased from 8.8 to 13.6 J kg^-1 K^-1 under applied magnetic field change of 5 T accompanying unobvious hysteresis and decreased magnetic transition temperature from 59 to 8 K, which is more promising as magnetic refrigerant at cryogenic temperature. This work provides a novel concept of designing heterogeneous structure in terms of special cluster and preferential nanocrystalline to modulate the properties of metallic glasses.

Key words: High-entropy metallic glass, Hydrogenation, Heterogeneous structure, Magnetocaloric effect

Liliang Shao, Lin Xue, Qiang Luo, Kuibo Yin, Zirui Yuan, Mingyun Zhu, Tao Liang, Qiaoshi Zeng, Litao Sun, Baolong Shen. Heterogeneous GdTbDyCoAl high-entropy alloy with distinctive magnetocaloric effect induced by hydrogenation[J]. J. Mater. Sci. Technol., 2022, 109: 147-156.

Figures/Tables 11

Fig. 1. (a) SEM image of the Gd20Tb18Dy18Co20Al24 amorphous powders. (b) XRD patterns of the GdTbDyCoAl and GdTbDyCoAlH powders.

Fig. 2. Isothermal magnetization curves for the (a) GdTbDyCoAl and (b) GdTbDyCoAlH powders.

Fig. 3. Temperature dependence of ΔSM under the maximum applied field from 0.5 to 5 T for the (a) GdTbDyCoAl and (b) GdTbDyCoAlH powders.

Fig. 4. Field dependence of ΔSM at different temperatures for the (a) GdTbDyCoAl and (b) GdTbDyCoAlH powders. (c) Temperature dependence of n values obtained from (a) and (b).

Fig. 5. (a) Magnetic hysteresis loops from -5 to 5 T at the temperature of 5 K for the two samples. Isothermal magnetizing and demagnetizing M-H curves at several temperatures below TM for the (b) GdTbDyCoAl and (c) GdTbDyCoAlH samples. (d) Temperature dependence of hysteretic loss.

Fig. 6. Arrott plots calculated from M-H curves for the (a) GdTbDyCoAl and (b) GdTbDyCoAlH powders. (c) and (d) The universal curves of ΔSM for the samples.

Fig. 7. Temperature dependence of magnetization under the applied magnetic field of 0.01 T for the GdTbDyCoAl and GdTbDyCoAlH powders. The inset shows the determination of TM and Curie-Weiss fitting.

Fig. 8. The real part of susceptibility (χ′) at frequency ranging from 13 to 9673 Hz for the (a) GdTbDyCoAl and (b) GdTbDyCoAlH samples. (c) The maximum relaxation time (τmax) versus the peak temperature of susceptibility (Tf) for the samples.

Fig. 9. HRTEM images and corresponding FFT patterns for (a)-(e) GdTbDyCoAl and (f)-(l) GdTbDyCoAlH samples, respectively.

Fig. 10. FFT patterns of the selected areas (C and D) in Fig. 9(a) and (g) for the (a) GdTbDyCoAl and (b) GdTbDyCoAlH samples. (c) and (d) showing the corresponding segmentation of the HRTEM image for auto-correlation analysis. The dimension of each cell is 1.98 × 1.98 nm2.

Fig. 11. Indentation load versus indentation depth of the 5 × 5 array for the (a) GdTbDyCoAl and (b) GdTbDyCoAlH powders, respectively. (c) and (d) Variations of the hardness (Hn) and reduced modulus (Er) obtained from the nanoindentation tests for the GdTbDyCoAl and GdTbDyCoAlH samples.

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