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设计制备具有优异形成能力和磁热效应的GdHoErCoNiAl高熵非晶合金

王壮 金凡 李伟 阮嘉艺 王龙飞 吴雪莲 张义坤 袁晨晨

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设计制备具有优异形成能力和磁热效应的GdHoErCoNiAl高熵非晶合金

王壮, 金凡, 李伟, 阮嘉艺, 王龙飞, 吴雪莲, 张义坤, 袁晨晨
cstr: 32037.14.aps.73.20241132

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
cstr: 32037.14.aps.73.20241132
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  • 通过对Gd, Ho和Er进行元素替换, 成功设计制备出临界尺寸为2 mm的Gd20+2xHo20–xEr20–xCo20Ni10Al10 (x = 0, 5, 10) 块体高熵非晶合金体系, 系统研究了稀土元素种类和含量对高熵非晶合金的微观结构、热力学性能和磁热性能的影响及调控机理. 研究结果表明, 随着Ho和Er逐步被Gd取代, 体系的热稳定性略有下降, 其中, 玻璃转变温度Tg和初始晶化温度Tx逐渐降低. 与此同时, 液相线温度Tl升高, 导致玻璃形成能力的热力学判据, 如约化玻璃转变温度Trg, γγm降低. X射线和高分辨透射电子显微镜的结果分析表明, 随着Gd含量的增大, 体系的有序度减小, 有利于非晶相的生成. 另一方面, 随着Gd元素的加入, 磁热性能参量如居里温度Tc、峰值磁熵变($ | {\Delta S_{\text{M}}^{{\text{pk}}}} | $)和相对制冷能力(relative cooling power, RCP)均逐渐升高, 其中Gd40Ho10Er10CoNiAl的$ | {\Delta S_{\text{M}}^{{\text{pk}}}} | $和RCP最大, 分别为8.31 J/(kg·K)和740.82 J/kg. 研究结果表明, 稀土基高熵非晶合金体系的磁热效应包括RCP, Tc和$ | {\Delta S_{\text{M}}^{{\text{pk}}}} | $主要依赖于de Gennes因子, 与材料内部的有效磁矩并无直接关系, 而热力学性能主要受到4f电子引起的f-d杂化效应影响, 随着4f电子数的增加非晶合金体系的热稳定逐步增加. 综上所述, 我们可以借助稀土元素替换进行成分优选, 通过调控4f电子数获得具有较高热稳定性且Tc可调的稀土基非晶合金磁热材料.
    In this work, Gd20+2xHo20–xEr20–xCo20Ni10Al10 (x = 0, 5, 10) high-entropy metallic glasses (MGs) with a critical diameter of 2 mm are successfully designed and fabricated by substituting Gd, Ho and Er. The effects of type and content of rare-earth (RE) elements on the microstructure, thermodynamic behaviors, and magnetocaloric effect (MCE) are investigated systematically. The amorphous structures of the ribbons and as-cast rods are confirmed by X-ray diffraction (XRD) with Cu Kα radiation (2θ = 20°–80°). The atomic-scale ordered configurations are examined by using high-resolution transmission electron microscope (HRTEM). Thermal analysis is carried out on differential scanning calorimeter (DSC) with a heating rate of 20 K/min by using ribbons. The magnetic measurements are conducted by using magnetometer in a temperature range of 5–180 K. According to DSC traces, it is suggested that as Ho and Er are replaced by Gd, the thermal stability of MGs slightly decreases, for example, both glass transition temperature (Tg) and initial crystallization temperature (Tx) decrease gradually, meanwhile the liquidus temperature (Tl) increases, which results in a reduction of glass-forming ability criteria such as the reduced glass transition temperatures Trg (Trg = Tg/Tl), γ (γ = Tx/(Tg + Tl)), and γm (γm = (2TxTg)/Tl), thermodynamically. The analyses based on XRD and HRTEM show that the degree of order in MGs decreases with Gd content increasing, which facilitates the glass formation. The magnetocaloric parameters such as Curie temperature (Tc), maximum magnetic entropy change ($ | {\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, Tc 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 Tc can be achieved by the RE substitution via adjusting the number of 4f electrons.
      通信作者: 袁晨晨, yuanchenchenneu@hotmail.com
    • 基金项目: 国家自然科学基金(批准号: 52071078)和东南大学至善学者A类项目(批准号: 2242021R41158)资助的课题.
      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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  • 图 1  Gd20+2xHo20–xEr20–xCoNiAl (x = 0, 5, 10)非晶合金条带(a)和铸棒(b)的XRD图谱

    Fig. 1.  XRD patterns of Gd20+2xHo20–xEr20–xCoNiAl (x = 0, 5, 10) ribbons (a) and rods (b).

    图 2  Gd20+2xHo20–xEr20–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

    Fig. 2.  (a)−(c) HRTEM image of Gd20+2xHo20–xEr20–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.

    图 3  (a) Gd20+2xHo20–xEr20–xCoNiAl (x = 0, 5, 10) 非晶合金条带DSC图; (b) TgTx与4f电子数的关系图

    Fig. 3.  (a) DSC traces of Gd20+2xHo20–xEr20–xCoNiAl (x = 0, 5, 10) ribbons; (b) Tg and Tx as a function of 4f electron number.

    图 4  (a) Gd20+2xHo20–xEr20–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) TcG因子的关系

    Fig. 4.  (a) Temperature dependence of ZFC and FC magnetization curves (M-T) of Gd20+2xHo20–xEr20–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) Tc as a function of G factor.

    图 5  Gd20+2xHo20–xEr20–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)

    Fig. 5.  Isothermal magnetization curves (M-H ) (a)–(c) and Arrott plots (d)–(f); magnetic entropy changes as a function of temperature (|ΔSM|-T ) (g)–(i) and $|\Delta S_{\text{M}}/ | {\Delta S_{\text{M}}^{{\text{pk}}}} |\text{-}\theta$ curves (j)–(l) for Gd20+2xHo20–xEr20–xCoNiAl (x = 0, 5, 10).

    图 6  Gd20+2xHo20–xEr20–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

    Fig. 6.  Magnetic entropy changes as a function of temperature (|ΔSM|-T) of Gd20+2xHo20–xEr20–xCoNiAl (x = 0, 5, 10) under an applied field of 5 T. The inset is RCP value.

    图 7  Gd20+2xHo20–xEr20–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

    Fig. 7.  Maximum magnetic entropy changes and relative cooling power as a function of applied field ($ | {\Delta S_{\text{M}}^{{\text{pk}}}} | $/RCP-H ) for Gd20+2xHo20–xEr20–xCoNiAl (x = 0, 5, 10). The solid lines are the exponential function fitting curves.

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

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

    图 9  (a) Tg, (b) Tx和(c) ΔTx与4f层电子数的关系

    Fig. 9.  (a) Tg, (b) Tx, and (c) ΔTx as a function of 4f electron number.

    表 1  Gd20+2xHo20–xEr20–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 Gd20+2xHo20–xEr20–xCoNiAl (x = 0, 5, 10).

    Compositions ΔSconf 4f electron number Tg/K Tx/K Tl/K ΔTx/K Trg γ γm
    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
    下载: 导出CSV

    表 2  Gd20+2xHo20–xEr20–xCoNiAl (x = 0, 5, 10)非晶合金的磁热参数

    Table 2.  Magnetocaloric parameters of Gd20+2xHo20–xEr20–xCoNiAl (x = 0, 5, 10).

    x
    ΔSconf G-factor Tc/K θ/K μeff/μB(实验) μeff/μB(理论) $ | {\Delta S_{\text{M}}^{{\text{pk}}}} | $/(J·kg–1·K–1) δTFWHM/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
    下载: 导出CSV
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出版历程
  • 收稿日期:  2024-08-14
  • 修回日期:  2024-09-10
  • 上网日期:  2024-09-27

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