Design and fabrication of GdHoErCoNiAl metallic glasses with excellent glass forming capability and magnetocaloric effects

Wang Zhuang; Jin Fan; Li Wei; Ruan Jia-Yi; Wang Long-Fei; Wu Xue-Lian; Zhang Yi-Kun; Yuan Chen-Chen

doi:10.7498/aps.73.20241132

Abstract

In this work, Gd_20+2xHo_20–xEr_20–xCo₂₀Ni₁₀Al₁₀ (x = 0, 5, 10) high-entropy metallic glasses (MGs) with a critical diameter of 2 mm are successfully designed and fabricated by substituting Gd, Ho and Er. The effects of type and content of rare-earth (RE) elements on the microstructure, thermodynamic behaviors, and magnetocaloric effect (MCE) are investigated systematically. The amorphous structures of the ribbons and as-cast rods are confirmed by X-ray diffraction (XRD) with Cu Kα radiation (2θ = 20°–80°). The atomic-scale ordered configurations are examined by using high-resolution transmission electron microscope (HRTEM). Thermal analysis is carried out on differential scanning calorimeter (DSC) with a heating rate of 20 K/min by using ribbons. The magnetic measurements are conducted by using magnetometer in a temperature range of 5–180 K. According to DSC traces, it is suggested that as Ho and Er are replaced by Gd, the thermal stability of MGs slightly decreases, for example, both glass transition temperature (T_g) and initial crystallization temperature (T_x) decrease gradually, meanwhile the liquidus temperature (T_l) increases, which results in a reduction of glass-forming ability criteria such as the reduced glass transition temperatures T_rg (T_rg = T_g/T_l), γ (γ = T_x/(T_g + T_l)), and γ_m (γ_m = (2T_x – T_g)/T_l), thermodynamically. The analyses based on XRD and HRTEM show that the degree of order in MGs decreases with Gd content increasing, which facilitates the glass formation. The magnetocaloric parameters such as Curie temperature (T_c), maximum magnetic entropy change ($ | {\Delta S_{\text{M}}^{{\text{pk}}}} | $) and relative cooling power (RCP) all increase gradually with the addition of Gd. The Gd₄₀Ho₁₀Er₁₀CoNiAl exhibits the best refrigeration performance in all studied systems, where the peak value of $ |{\Delta S}_{{\mathrm{M}}}| $ is 8.31 J/(kg·K) and RCP is 740.82 J/kg. The results indicate that MCEs of MGs including RCP, T_c and $ | {\Delta S_{\text{M}}^{{\text{pk}}}} | $, mainly depend on the de Gennes factor rather than the effective magnetic moment, while thermodynamic properties are more affected by the f-d hybridization effect. As the number of 4f electrons increases, the thermal stability increases with the degree f-d orbital hybridization increasing. In summary, the RE-based MG with high thermal stability and adjustable T_c can be achieved by the RE substitution via adjusting the number of 4f electrons.

Keywords:

rare-earth based high-entropy metallic glasses /
thermodynamic properties /
magnetocaloric effect /
glass forming ability

Authors and contacts

1.
School of Materials Science and Engineering, Southeast University, Nanjing 211189, China
2.
School of Materials and Environmental Engineering, Hangzhou Dianzi University, Hangzhou 310018, China
3.
School of Materials Science and Engineering, Anhui University of Technology, Ma'anshan 243032, China

Corresponding author: Yuan Chen-Chen, yuanchenchenneu@hotmail.com

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 52071078) and the “Zhishan” Scholars Programs of Southeast University, China (Grant No. 2242021R41158).

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Cited By

图 1 Gd_20+2xHo_20–xEr_20–xCoNiAl (x = 0, 5, 10)非晶合金条带(a)和铸棒(b)的XRD图谱

Figure 1. XRD patterns of Gd_20+2xHo_20–xEr_20–xCoNiAl (x = 0, 5, 10) ribbons (a) and rods (b).

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图 2 Gd_20+2xHo_20–xEr_20–xCoNiAl (x = 0, 5, 10)非晶合金条带HRTEM图(a)—(c)及选区二维自相关处理图(d)—(f), 插图为选区电子衍射图

Figure 2. (a)−(c) HRTEM image of Gd_20+2xHo_20–xEr_20–xCoNiAl (x = 0, 5, 10) ribbons and (d)−(f) 2D auto-correlation processing image of selected area. The inset shows the selected area electron diffraction pattern.

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图 3 (a) Gd_20+2xHo_20–xEr_20–xCoNiAl (x = 0, 5, 10) 非晶合金条带DSC图; (b) T_g和T_x与4f电子数的关系图

Figure 3. (a) DSC traces of Gd_20+2xHo_20–xEr_20–xCoNiAl (x = 0, 5, 10) ribbons; (b) T_g and T_x as a function of 4f electron number.

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图 4 (a) Gd_20+2xHo_20–xEr_20–xCoNiAl (x = 0, 5, 10)非晶合金200 Oe外场场冷和零场冷磁化强度与温度关系图; (b) 200 Oe外场下的$ {1 {/ } {\chi \left( T \right)}} $随温度变化曲线; (c)场冷曲线求导图; (d) T_c与G因子的关系

Figure 4. (a) Temperature dependence of ZFC and FC magnetization curves (M-T) of Gd_20+2xHo_20–xEr_20–xCoNiAl (x = 0, 5, 10) under 200 Oe; (b) $ {1 {/ } {\chi \left( T \right)}} $ curves at H = 200 Oe; (c) dM/dT-T curves; (d) T_c as a function of G factor.

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图 5 Gd_20+2xHo_20–xEr_20–xCoNiAl (x = 0, 5, 10)非晶合金不同温度下磁化强度与外场关系图(a)—(c)和Arrott图(d)—(f); 不同外场下的磁熵变与温度关系图(g)—(i)和$|\Delta S_{\text{M}}/ | {\Delta S_{\text{M}}^{{\text{pk}}}} |\text{-}\theta$图(j)—(l)

Figure 5. Isothermal magnetization curves (M-H ) (a)–(c) and Arrott plots (d)–(f); magnetic entropy changes as a function of temperature (|ΔS_M|-T ) (g)–(i) and $|\Delta S_{\text{M}}/ | {\Delta S_{\text{M}}^{{\text{pk}}}} |\text{-}\theta$ curves (j)–(l) for Gd_20+2xHo_20–xEr_20–xCoNiAl (x = 0, 5, 10).

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图 6 Gd_20+2xHo_20–xEr_20–xCoNiAl (x = 0, 5, 10)非晶合金5 T外场下磁熵变与温度关系图, 插图为3种合金相对制冷量值

Figure 6. Magnetic entropy changes as a function of temperature (|ΔS_M|-T) of Gd_20+2xHo_20–xEr_20–xCoNiAl (x = 0, 5, 10) under an applied field of 5 T. The inset is RCP value.

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图 7 Gd_20+2xHo_20–xEr_20–xCoNiAl (x = 0, 5, 10)非晶合金(a)峰值磁熵变和(b)相对制冷能力与外场关系图, 实线为指数函数拟合曲线

Figure 7. (a) Maximum magnetic entropy changes and (b) relative cooling power as a function of applied field ($ | {\Delta S_{\text{M}}^{{\text{pk}}}} | $/RCP-H ) for Gd_20+2xHo_20–xEr_20–xCoNiAl (x = 0, 5, 10). The solid lines are the exponential function fitting curves.

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图 8 (a) T_c, (b) $ | {\Delta S_{\text{M}}^{{\text{pk}}}} | $和(c) RCP与G因子的关系

Figure 8. (a) T_c, (b) $ | {\Delta S_{\text{M}}^{{\text{pk}}}} | $, and (c) RCP as a function of G factor.

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图 9 (a) T_g, (b) T_x和(c) ΔT_x与4f层电子数的关系

Figure 9. (a) T_g, (b) T_x, and (c) ΔT_x as a function of 4f electron number.

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表 1 Gd_20+2xHo_20–xEr_20–xCoNiAl (x = 0, 5, 10)非晶合金热力学参数(R为气体常数)

Table 1. Thermodynamic parameters and GFA criteria of Gd_20+2xHo_20–xEr_20–xCoNiAl (x = 0, 5, 10).

Compositions	ΔS_conf	4f electron number	T_g/K	T_x/K	T_l/K	ΔT_x/K	T_rg	γ	γ_m
x = 0	1.748R	9.33	560.6	616.3	973.0	55.7	0.576	0.402	0.691
x = 5	1.713R	8.75	554.8	613.9	989.6	59.1	0.561	0.398	0.680
x = 10	1.609R	8.17	551.3	605.3	985.6	54.0	0.559	0.394	0.669

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表 2 Gd_20+2xHo_20–xEr_20–xCoNiAl (x = 0, 5, 10)非晶合金的磁热参数

Table 2. Magnetocaloric parameters of Gd_20+2xHo_20–xEr_20–xCoNiAl (x = 0, 5, 10).

x	ΔS_conf	G-factor	T_c/K	θ/K	μ_eff/μ_B(实验)	μ_eff/μ_B(理论)	$ \| {\Delta S_{\text{M}}^{{\text{pk}}}} \| $/(J·kg^–1·K^–1)	δT_FWHM/K	RCP/(J·kg^–1)	n	N
0	1.748R	7.60	65	17.968	7.18	7.75	8.21	73.99	607.20	0.80	1.00
5	1.713R	9.64	67	77.788	6.68	7.45	8.28	80.43	665.67	0.78	1.00
10	1.609R	11.68	81	92.191	6.61	7.14	8.31	89.17	740.82	0.76	1.01

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