纳米复合MgAgSb基合金的热电输运性能优化

doi:10.15541/jim20250010

无机材料学报 ›› 2025, Vol. 40 ›› Issue (9): 997-1004.DOI: 10.15541/jim20250010

纳米复合MgAgSb基合金的热电输运性能优化

吴华鑫¹(), 张骐昊², YAN Haixue³, 王连军¹(), 江莞¹^,²

1.东华大学材料科学与工程学院, 先进纤维材料全国重点实验室, 上海 201620
2.东华大学功能材料研究中心, 上海 201620
3. School of Engineering and Materials Science, Queen Mary University of London, London E1 4NS, UK

收稿日期:2025-01-08 修回日期:2025-03-29 出版日期:2025-09-20 网络出版日期:2025-04-09
通讯作者: 王连军, 教授. E-mail: wanglj@dhu.edu.cn
作者简介:吴华鑫(2000-), 男, 硕士研究生. E-mail: wuhuaxin2163@163.com
基金资助:
国家自然科学基金(U23A20685);上海市教委科研创新项目(2021-01-07-00-03-E00110);上海市科委项目(23520710300)

Optimization of Thermoelectric Transport Properties in Nanocomposite MgAgSb-based Alloys

WU Huaxin¹(), ZHANG Qihao², YAN Haixue³, WANG Lianjun¹(), JIANG Wan¹^,²

1. State Key Laboratory of Advanced Fiber Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, China
2. China Institute of Functional Materials, Donghua University, Shanghai 201620, China
3. School of Engineering and Materials Science, Queen Mary University of London, London E1 4NS, UK

Received:2025-01-08 Revised:2025-03-29 Published:2025-09-20 Online:2025-04-09
Contact: WANG Lianjun, professor. E-mail: wanglj@dhu.edu.cn
About author:WU Huaxin (2000-), male, Master candidate. E-mail: wuhuaxin2163@163.com
Supported by:
National Natural Science Foundation of China(U23A20685);Innovation Program of Shanghai Municipal Education Commission(2021-01-07-00-03-E00110);Shanghai Science and Technology Commission Project(23520710300)

摘要/Abstract

摘要：

MgAgSb在近室温区间(300~573 K)表现出良好的热电性能, 近年来成为p型材料的重点研究对象。由于原子掺杂水平较低, 仅采用掺杂手段优化载流子浓度, 热电性能的增幅有限。本研究选择在MgAg_0.97Sb_0.99基体材料中分别引入Nb和Ta纳米第二相, 通过高能球磨机械合金化的方法制备了xNb/MgAg_0.97Sb_0.99和yTa/MgAg_0.97Sb_0.99两种系列合金。引入Nb纳米第二相显著改变了材料的载流子和声子输运特性。0.005Nb/MgAg_0.97Sb_0.99合金中由于存在纳米第二相Nb, 其特殊的微观结构优化了电学性能, 该合金在533 K时的最高功率因子为24.1 μW·cm^-1·K^-2。同时, 引入的Nb第二相增加了声子散射, 从而显著降低了热导率, 最终0.005Nb/MgAg_0.97Sb_0.99样品的热电优值(zT)在483 K时达到最大1.09, 相较于MgAg_0.97Sb_0.99样品提升了9.0%。此外, 在MgAg_0.97Sb_0.99样品中引入Nb的同族元素Ta, 其产生的影响与Nb近似, 0.005Ta/MgAg_0.97Sb_0.99样品在483 K时zT达到1.02。本研究展示了一种有效的纳米复合策略, 能够优化热电输运性能并提高p型MgAg_0.97Sb_0.99的热电性能。

关键词: MgAgSb基化合物, 第二相, 合金化, 热电性能

Abstract:

MgAgSb exhibits excellent thermoelectric performance in the near-room temperature range of 300-573 K, making it a key research focus for p-type materials in recent years. Due to the low level of atomic doping, the improvement of thermoelectric performance through carrier concentration optimization via doping alone is limited. In this study, Nb and Ta nano-secondary phases were introduced into the MgAg_0.97Sb_0.99 matrix, and two series of alloys, xNb/MgAg_0.97Sb_0.99 and yTa/MgAg_0.97Sb_0.99, were prepared using high-energy ball milling mechanical alloying. The introduction of Nb nano-secondary phase significantly altered carrier and phonon transport properties of the material. It was the presence of nano-secondary phase Nb in the 0.005Nb/MgAg_0.97Sb_0.99 alloy that optimized its unique microstructure and electrical performance, achieving a maximum power factor of 24.1 μW·cm^-1·K^-2 at 533 K. Additionally, the introduction of secondary phase enhanced phonon scattering, significantly reducing thermal conductivity. As a result, the 0.005Nb/MgAg_0.97Sb_0.99 sample achieved an optimal zT of 1.09 at 483 K, improved by 9.0% compared to MgAg_0.97Sb_0.99 at the same temperature. Furthermore, the introduction of Ta, a homologue of Nb, into the MgAg_0.97Sb_0.99 sample showed a similar trend, with 0.005Ta/MgAg_0.97Sb_0.99 achieving zT of 1.02 at 483 K. This study demonstrates an effective nanocomposite strategy for optimizing thermoelectric transport properties and enhancing thermoelectric performance of p-type MgAg_0.97Sb_0.99.

Key words: MgAgSb-based compound, secondary phase, alloying, thermoelectric performance

中图分类号:

TQ174

吴华鑫, 张骐昊, YAN Haixue, 王连军, 江莞. 纳米复合MgAgSb基合金的热电输运性能优化[J]. 无机材料学报, 2025, 40(9): 997-1004.

WU Huaxin, ZHANG Qihao, YAN Haixue, WANG Lianjun, JIANG Wan. Optimization of Thermoelectric Transport Properties in Nanocomposite MgAgSb-based Alloys[J]. Journal of Inorganic Materials, 2025, 40(9): 997-1004.

图/表 6

图1 xNb/MgAg0.97Sb0.99样品的物相组成

Fig. 1 Phase compositions of xNb/MgAg0.97Sb0.99 samples (a) XRD patterns; (b-d) Surface scan element distributions of xNb/MgAg0.97Sb0.99 samples when x is (b) 0.005, (c) 0.010, and (d) 0.015

图2 xNb/MgAg0.97Sb0.99合金的电输运性能

Fig. 2 Electrical properties of xNb/MgAg0.97Sb0.99 alloys (a) Nb content dependent room-temperature carrier concentration and mobility; (b-d) Temperature dependence of (b) electrical conductivity, (c) Seebeck coefficient, and (d) power factor

图3 xNb/MgAg0.97Sb0.99合金的热输运性能及热电优值随温度的变化关系

Fig. 3 Temperature dependence of thermal properties and figure of merit for xNb/MgAg0.97Sb0.99 alloys (a) Total thermal conductivity; (b) Thermal conductivity comprising lattice and bipolar contributions; (c) zT; (d) Comparison of peak zT and average zT. Colorful figures are available on website

图4 yTa/MgAg0.97Sb0.99样品的物相组成

Fig. 4 Phase compositions of yTa/MgAg0.97Sb0.99 samples (a) XRD patterns; (b-d) Surface scan element distributions of yTa/MgAg0.97Sb0.99 samples when y is (b) 0.005, (c) 0.010, and (d) 0.015

图5 yTa/MgAg0.97Sb0.99合金的电输运性能

Fig. 5 Electrical properties for yTa/MgAg0.97Sb0.99 alloys (a) Ta content dependent room-temperature carrier concentration and mobility; (b-d) Temperature dependence of (b) electrical conductivity, (c) Seebeck coefficient, and (d) power factor

图6 yTa/MgAg0.97Sb0.99合金的热输运性能及热电优值随温度的变化关系

Fig. 6 Temperature dependence of thermal properties and figure of merit for yTa/MgAg0.97Sb0.99 alloys (a) Total thermal conductivity; (b) Thermal conductivity comprising lattice and bipolar contributions; (c) zT; (d) Comparison between peak zT and average zT. Colorful figures are available on website

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纳米复合MgAgSb基合金的热电输运性能优化

Optimization of Thermoelectric Transport Properties in Nanocomposite MgAgSb-based Alloys

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