Pd基非晶合金动态弛豫机制和应力松弛行为

段亚娟; 乔吉超

doi:10.7498/aps.71.20212025

摘要

作为潜在的功能及结构材料, 高熵非晶合金在凝聚态物理和力学领域引起广泛的研究兴趣. 高熵非晶合金宏观力学性能与微观结构非均匀性之间的关联是当前重要的科学问题之一. 本文选取非晶形成能力良好的Pd_42.5Cu₃₀Ni_7.5P₂₀非晶合金和Pd₂₀Pt₂₀Cu₂₀Ni₂₀P₂₀高熵非晶合金作为模型体系, 借助于动态弛豫行为及应力松弛实验建立了温度和物理时效对非晶合金高温变形机制与微观结构非均匀性之间的关联. 研究结果表明Pd基非晶合金表现出“肩膀峰”β弛豫形式. 玻璃转变温度以下物理时效非晶合金体系原子移动性导致β弛豫肩膀峰往更高的温度迁移. 在应力松弛过程中, 由于高构型熵的引入降低吉布斯自由能, 这是高熵非晶合金具有较高激活能的原因. 高熵非晶合金更难被激活, 需要突破更高的能量势垒. 物理时效时间增加, 高熵非晶合金流变单元更小, 这也得益于多主元高熵非晶合金慢扩散效应. 高熵非晶合金激活体积的改变在物理时效下应力松弛过程中的敏感性低于对应的非晶合金.

关键词:

Abstract

As a potential functional and structural material, high-entropy metallic glasses have aroused tremendous research interest in condense matter physics and mechanics. The correlation between macroscopic mechanic properties and microstructure heterogeneity of high-entropy metallic glasses is one of the most important scientific issues in glassy solids. In the present research, Pd_42.5Cu₃₀Ni_7.5P₂₀ metallic glass and Pd₂₀Pt₂₀Cu₂₀Ni₂₀P₂₀ high-entropy metallic glass are selected as the model alloys. Dynamic mechanical analysis (DMA) and stress relaxation are used to investigate the influences of temperature and physical aging on dynamic mechanical relaxation process and microstructure heterogeneity of the model alloys. The dynamic mechanical analysis results demonstrate that the Pd_42.5Cu₃₀Ni_7.5P₂₀ metallic glass and Pd₂₀Pt₂₀Cu₂₀Ni₂₀P₂₀ high-entropy metallic glass both exhibit evident β relaxation process. In addition, the atomic mobility of model alloys is reduced in these processes, and the β relaxation shifts toward higher temperatures. In the stress relaxation process, the Gibbs free energy is reduced due to the high configurational entropy. This is the potential reason that high-entropy metallic glass possesses higher activation energy. In parallel, high-entropy metallic glass is more difficult to activate and needs to break through a higher energy barrier. With the increase of physical aging time, the flow unit in high-entropy metallic glass becomes smaller. This also benefits from the high-entropy effects that bring sluggish diffusion into high-entropy metallic glass. The change of activation volume under physical aging of high-entropy metallic glass is less sensitive to stress relaxation than that of metallic glass.

Keywords:

作者及机构信息

西北工业大学力学与土木建筑学院, 西安　710072

通信作者: 乔吉超, qjczy@nwpu.edu.cn

基金项目: 国家自然科学基金 (批准号: 51971178)、陕西省杰出青年基金(批准号: 2021JC-12)和西北工业大学博士论文创新基金(批准号: CX202031)资助的课题.

Authors and contacts

School of Mechanics, Civil Engineering and Architecture, Northwestern Polytechnical University, Xi’an 710072, China

Corresponding author: Qiao Ji-Chao, qjczy@nwpu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 51971178), the Natural Science Basic Research Plan for Distinguished Young Scholars in Shaanxi Province, China (Grant No. 2021JC-12), and the Innovation Foundation for Doctoral Dissertation of Northwestern Polytechnical University, China (Grant No. CX202031).

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参考文献

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施引文献

图 1 Pd_42.5Cu₃₀Ni_7.5P₂₀非晶合金和Pd₂₀Pt₂₀Cu₂₀Ni₂₀P₂₀高熵非晶合金DSC曲线(升温速率为20 K/min). 玻璃转变温度$ {T_{\text{g}}} $和晶化温度$ {T_{\text{x}}} $如图中箭头所示

Fig. 1. DSC curves of Pd_42.5Cu₃₀Ni_7.5P₂₀ metallic glass and Pd₂₀Pt₂₀Cu₂₀Ni₂₀P₂₀ high-entropy metallic glass with a heating rate of 20 K/min. The glass transition temperature $ {T_{\text{g}}} $ and the onset crystallization temperature $ {T_{\text{x}}} $ are shown by the arrows.

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图 2 (a) Pd_42.5Cu₃₀Ni_7.5P₂₀非晶合金和 (b) Pd₂₀Pt₂₀Cu₂₀Ni₂₀P₂₀高熵非晶合金铸态^[38]时效后归一化损耗模量${E''}/E_{\max }''$随归一化温度$ T/{T_\alpha } $的演化($E_{\max }''$为两种模型合金损耗模量最大值, $ {T_\alpha } $为两种模型合金α弛豫的峰值温度), 升温速率为 3 K/min, 加载频率为3 Hz. 物理时效温度为0.824$ {T_{\text{g}}} $

Fig. 2. Evolution of the normalized loss modulus ${E''}/E_{\max }''$of (a) Pd_42.5Cu₃₀Ni_7.5P₂₀ metallic glass and (b) Pd₂₀Pt₂₀Cu₂₀Ni₂₀P₂₀ high-entropy metallic glass ^[38] as a function of normalized temperature $ T/{T_\alpha } $ with the state of as-cast and pre-aging (aging temperature is 0.824$ {T_{\text{g}}} $). The driving frequency is 3 Hz, the heating rate is 3 K/min and $ {T_\alpha } $ is the peak temperature of α relaxation.

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图 3 (a) Pd_42.5Cu₃₀Ni_7.5P₂₀非晶合金和(b) Pd₂₀Pt₂₀Cu₂₀Ni₂₀P₂₀高熵非晶合金在不同温度下(0.8$ {T_{\text{g}}} $—0.9$ {T_{\text{g}}} $)的应力松弛行为, 应力通过初始应力进行归一化, 实线是KWW方程拟合曲线

Fig. 3. Stress relaxation spectra of (a) Pd_42.5Cu₃₀Ni_7.5P₂₀ metallic glass and (b) Pd₂₀Pt₂₀Cu₂₀Ni₂₀P₂₀ high-entropy metallic glass at different temperatures. KWW fittings are shown with solid lines.

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图 4 Pd_42.5Cu₃₀Ni_7.5P₂₀非晶合金和Pd₂₀Pt₂₀Cu₂₀Ni₂₀P₂₀高熵非晶合金拟合参数　(a) $ {\beta _{{\text{KWW}}}} $, (b) $ n $随温度的演化

Fig. 4. Fitting parameters (a) $ {\beta _{{\text{KWW}}}} $, (b) $ n $ of Pd_42.5Cu₃₀Ni_7.5P₂₀ metallic glass and Pd₂₀Pt₂₀Cu₂₀Ni₂₀P₂₀ high-entropy metallic glass as a function of temperature.

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图 5 Pd_42.5Cu₃₀Ni_7.5P₂₀非晶合金和Pd₂₀Pt₂₀Cu₂₀Ni₂₀P₂₀高熵非晶合金应力松弛弛豫时间$ {\tau _{\text{c}}} $随温度的演化. 直线为基于Arrhenius公式拟合

Fig. 5. Dependence of the characteristic stress relaxation time $ {\tau _{\text{c}}} $ on the reciprocal stress relaxation temperature T_g/T of Pd_42.5Cu₃₀Ni_7.5P₂₀ metallic glass and Pd₂₀Pt₂₀Cu₂₀Ni₂₀P₂₀ high-entropy metallic glass. The solid lines are the fittings with Arrhenius equation.

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图 6 (a) Pd_42.5Cu₃₀Ni_7.5P₂₀非晶合金和 (b) Pd₂₀Pt₂₀Cu₂₀Ni₂₀P₂₀高熵非晶合金在0.824$ {T_{\text{g}}} $时效1800, 3600, 7200, 10800 s后的应力松弛谱及拟合曲线

Fig. 6. Stress relaxation and the corresponding fitting curves for (a) Pd_42.5Cu₃₀Ni_7.5P₂₀ metallic glass and (b) Pd₂₀Pt₂₀Cu₂₀Ni₂₀P₂₀ high-entropy metallic glass after different aging time (1800, 3600, 7200, 10800 s) at 0.824$ {T_{\text{g}}} $.

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图 7 Pd_42.5Cu₃₀Ni_7.5P₂₀非晶合金和 Pd₂₀Pt₂₀Cu₂₀Ni₂₀P₂₀高熵非晶合金拟合参数　(a) $ n $, (b) $ {V_{\text{a}}} $, (c) $ {C_{\text{r}}} $随物理时效时间的演化

Fig. 7. The fitting parameters (a) $ n $, (b) $ {V_{\text{a}}} $, (c) $ {C_{\text{r}}} $of Pd_42.5Cu₃₀Ni_7.5P₂₀ metallic glass and Pd₂₀Pt₂₀Cu₂₀Ni₂₀P₂₀ high-entropy metallic glass as a function of aging time.

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图 8 (a) Pd_42.5Cu₃₀Ni_7.5P₂₀非晶合金和 (b) Pd₂₀Pt₂₀Cu₂₀Ni₂₀P₂₀高熵非晶合金激活能谱随时效时间的演化

Fig. 8. Evolution of activation energy spectrum of (a) Pd_42.5Cu₃₀Ni_7.5P₂₀ metallic glass and (b) Pd₂₀Pt₂₀Cu₂₀Ni₂₀P₂₀ high-entropy metallic glass with different aging time.

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[36]	Yang M, Liu X, Ruan H, Wu Y, Wang H, Lu Z 2016 J. Appl. Phys. 119 245112 Google Scholar
[37]	Zhang L, Duan Y, Crespo D, Pineda E, Wada T, Kato H, Pelletier J M, Qiao J 2021 Appl. Phys. Lett. 119 051905 Google Scholar
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Pd基非晶合金动态弛豫机制和应力松弛行为