熵调控抑制ZrNiSn基half-Heusler热电材料的晶格热导率

doi:10.15541/jim20210610

无机材料学报 ›› 2022, Vol. 37 ›› Issue (7): 717-723.DOI: 10.15541/jim20210610

所属专题：【结构材料】高熵陶瓷；【能源环境】热电材料

熵调控抑制ZrNiSn基half-Heusler热电材料的晶格热导率

王鹏将¹(), 康慧君¹(), 杨雄¹, 刘颖², 程成¹, 王同敏¹

1.大连理工大学材料科学与工程学院, 辽宁省凝固控制与数字化制备技术重点实验室, 大连116024
2.大连理工大学三束材料改性教育部重点实验室, 大连116024

收稿日期:2021-10-05 修回日期:2021-11-28 出版日期:2022-07-20 网络出版日期:2021-12-02
通讯作者: 康慧君, 教授. E-mail: kanghuijun@dlut.edu.cn
作者简介:王鹏将(1996-), 男, 硕士研究生. E-mail: wpj@mail.dlut.edu.cn
基金资助:
国家自然科学基金(51971052);国家自然科学基金(51774065);辽宁省“兴辽英才计划”(XLYC2007183);辽宁省“兴辽英才计划”(XLYC1808005);大连市科技创新基金(2020JJ25CY002);大连市科技创新基金(2020JJ26GX045)

Inhibition of Lattice Thermal Conductivity of ZrNiSn-based Half-Heusler Thermoelectric Materials by Entropy Adjustment

WANG Pengjiang¹(), KANG Huijun¹(), YANG Xiong¹, LIU Ying², CHENG Cheng¹, WANG Tongmin¹

1. Key Laboratory of Solidification Control and Digital Preparation Technology (Liaoning Province), School of Materials Science and Engineering, Dalian University of Technology, Dalian 116024, China
2. Key Laboratory of Material Modification by Laser, Ion and Electron Beams, Ministry of Education, Dalian University of Technology, Dalian 116024, China

Received:2021-10-05 Revised:2021-11-28 Published:2022-07-20 Online:2021-12-02
Contact: KANG Huijun, professor. E-mail: kanghuijun@dlut.edu.cn
About author:WANG Pengjiang (1996-), male, Master candidate. E-mail: wpj@mail.dlut.edu.cn
Supported by:
National Natural Science Foundation of China(51971052);National Natural Science Foundation of China(51774065);Liaoning Revitalization Talents Program(XLYC2007183);Liaoning Revitalization Talents Program(XLYC1808005);Innovation Foundation of Science and Technology of Dalian(2020JJ25CY002);Innovation Foundation of Science and Technology of Dalian(2020JJ26GX045)

摘要/Abstract

摘要：

ZrNiSn基half-Heusler热电材料具有较高的热导率, 限制了其热电性能进一步提高。为了降低晶格热导率, 本研究采用磁悬浮熔炼和放电等离子烧结的方法制备ZrNiSn和Zr_0.5Hf_0.5Ni_1-_xPt_xSn (x=0, 0.1, 0.15, 0.2, 0.25, 0.3)高熵half-Heusler热电合金。在Zr位进行Hf原子替代, Ni位进行Pt原子替代以调控该合金的构型熵, 并研究构型熵对热电性能的影响。本工作优化了Zr_0.5Hf_0.5Ni_0.85Pt_0.15Sn在673 K的最小晶格热导率和双极扩散热导率之和为2.1 W·m^-1·K^-1, 与ZrNiSn相比降低了约58%。这一发现为降低ZrNiSn基合金的晶格热导率提供了一种有效的策略, 有助于改善材料的热电性能。

关键词: 高熵, half-Heusler合金, 热电材料, 晶格热导率

Abstract:

The thermoelectric properties of ZrNiSn-based half-Heusler materials were hindered due to their high thermal conductivity. In order to reduce the lattice thermal conductivity, the high-entropy alloys ZrNiSn and Zr_0.5Hf_0.5Ni_1-_xPt_xSn (x=0, 0.1, 0.15, 0.2, 0.25, 0.3) were prepared by levitation melting and spark plasma sintering. Configurational entropy of the alloys was manipulated by Hf substitution for Zr and Pt substitution for Ni. Effects of configuration entropy on the thermoelectric properties were investigated. The reslults showed that the minimum sum of lattice thermal conductivity and bipolar thermal conductivity (κ_l+κ_b) at 673 K for Zr_0.5Hf_0.5Ni_0.85Pt_0.15Sn was optimized at 2.1 W·m^-1·K^-1, which was significantly reduced by about 58% when compared with ZrNiSn. This finding provides an effective strategy for reducing lattice thermal conductivity of ZrNiSn-based alloy to offer great potential for further improvement of thermoelectrics.

Key words: high entropy, half-Heusler alloy, thermoelectric material, lattice thermal conductivity

中图分类号:

O472

王鹏将, 康慧君, 杨雄, 刘颖, 程成, 王同敏. 熵调控抑制ZrNiSn基half-Heusler热电材料的晶格热导率[J]. 无机材料学报, 2022, 37(7): 717-723.

WANG Pengjiang, KANG Huijun, YANG Xiong, LIU Ying, CHENG Cheng, WANG Tongmin. Inhibition of Lattice Thermal Conductivity of ZrNiSn-based Half-Heusler Thermoelectric Materials by Entropy Adjustment[J]. Journal of Inorganic Materials, 2022, 37(7): 717-723.

图/表 7

图1 ZrNiSn和Zr0.5Hf0.5Ni1-xPtxSn的XRD图谱

Fig. 1 XRD patterns of ZrNiSn and Zr0.5Hf0.5Ni1-xPtxSn

图2 Zr0.5Hf0.5Ni1-xPtxSn的二次电子照片

Fig. 2 Secondary electron images of Zr0.5Hf0.5Ni1-xPtxSn (a) x=0; (b) x=0.1; (c) x=0.15; (d) x=0.2; (e) x=0.25; (f) x=0.3

图3 Zr0.5Hf0.5Ni0.85Pt0.15Sn试样的元素面扫描EPMA图

Fig. 3 EPMA elemental mappings of nominal Zr0.5Hf0.5Ni0.85Pt0.15Sn sample

图4 ZrNiSn和Zr0.5Hf0.5Ni1-xPtxSn试样的(a)电导率与温度的变化关系, (b)室温载流子浓度和迁移率与Pt掺杂量的变化关系, (c)Seebeck系数和(d)功率因子与温度的变化关系

Fig. 4 (a) Temperature dependence of electrical conductivity, (b) room temperature carrier concentration and carrier mobility varied with Pt content, temperature dependence of (c) Seebeck coefficient and (d) power factor of ZrNiSn and Zr0.5Hf0.5Ni1-xPtxSn

图5 ZrNiSn和Zr0.5Hf0.5Ni1-xPtxSn试样的(a)热扩散系数和(b)比热容与温度的变化关系

Fig. 5 Temperature dependence of (a) thermal diffusivity and (b) specific heat capacity for ZrNiSn and Zr0.5Hf0.5Ni1-xPtxSn samples

图6 (a)ZrNiSn和Zr0.5Hf0.5Ni1-xPtxSn试样总热导率与温度的变化关系, (b) 923 K时(κl+κb)随构型熵的变化关系, (c) (κl+κb)与温度的变化关系, (d) 不同样品的(κl+κb)的对比[17,23-24,35]

Fig. 6 (a) Temperature dependence of total thermal conductivity, (b) change of lattice thermal conductivity with configuration entropy at 923 K, (c) temperature dependence of lattice thermal conductivity of Zr0.5Hf0.5Ni1-xPtxSn (x=0, 0.1, 0.15, 0.2, 0.25, 0.3), and (d) comparison of lattice thermal conductivity of different samples [17,23-24,35]

图7 ZrNiSn和Zr0.5Hf0.5Ni1-xPtxSn试样的ZT

Fig. 7 ZT of ZrNiSn and Zr0.5Hf0.5Ni1-xPtxSn samples

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熵调控抑制ZrNiSn基half-Heusler热电材料的晶格热导率

Inhibition of Lattice Thermal Conductivity of ZrNiSn-based Half-Heusler Thermoelectric Materials by Entropy Adjustment

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