Mg含量对Mg3(1+z)Sb2化合物热电传输性能的影响

doi:10.15541/jim20200538

无机材料学报 ›› 2021, Vol. 36 ›› Issue (8): 835-840.DOI: 10.15541/jim20200538

所属专题：【虚拟专辑】热电材料(2020~2021)

Mg含量对Mg₃₍₁₊_z₎Sb₂化合物热电传输性能的影响

逯旭¹^,²(), 侯绩翀¹, 张强¹^,²(), 樊建锋¹, 陈少平², 王晓敏¹^,²()

1. 新材料界面科学与工程教育部重点实验室, 太原理工大学, 太原 030024
2.材料科学与工程学院, 太原 030024, 太原理工大学, 太原 030024

收稿日期:2020-09-15 修回日期:2020-11-04 出版日期:2021-08-20 网络出版日期:2020-12-01
通讯作者: 张强, 副教授. E-mail:zhangqiang@tyut.edu.cn; 王晓敏, 教授. E-mail:wangxiaomin@tyut.edu.cn
作者简介:逯旭(1995-), 男, 硕士研究生. E-mail: lx1486479798@163.com
基金资助:
国家自然科学基金(51601123);国家自然科学基金(U1710118);山西省自然科学基金(201801D221139);山西省高等学校科技创新计划(2019L0330)

Effect of Mg Content on Thermoelectric Property of Mg₃₍₁₊_z₎Sb₂ Compounds

LU Xu¹^,²(), HOU Jichong¹, ZHANG Qiang¹^,²(), FAN Jianfeng¹, CHEN Shaoping², WANG Xiaomin¹^,²()

1. Key Laboratory of Interface Science and Engineering in Advanced Materials, Ministry of Education, Taiyuan University of Technology, Taiyuan 030024, China
2. College of Materials Science and Engineering, Taiyuan University of Technology, Taiyuan 030024, China

Received:2020-09-15 Revised:2020-11-04 Published:2021-08-20 Online:2020-12-01
Contact: ZHANG Qiang, associate professor. E-mail:zhangqiang@tyut.edu.cn; WANG Xiaomin, professor. E-mail:wangxiaomin@tyut.edu.cn
About author:LU Xu(1995-), male, Master candidate. E-mail: lx1486479798@163.com
Supported by:
National Natural Science Foundation of China(51601123);National Natural Science Foundation of China(U1710118);Natural Science Foundation of Shanxi Province(201801D221139);Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi(2019L0330)

摘要/Abstract

摘要：

Mg₃Sb₂化合物具有良好的热电性能和成本优势, 受到研究者的广泛关注。由于Mg元素具有很高的饱和蒸汽压和化学反应活性, 因此Mg₃Sb₂在合成过程中含量难以精确控制。本研究利用固相反应/球磨结合放电等离子体烧结制备了不同Mg含量的Mg₃₍₁₊_z₎Sb₂(z=0, 0.02, 0.04, 0.06和0.08)样品, 通过物相结构分析和热电性能测试, 研究了Mg含量对Mg₃Sb₂化合物热电性能的影响规律。结果表明, 随着名义Mg含量的增加, 实际Mg含量在Mg₃Sb₂化合物中由缺失状态转变为过量状态, Mg₃₍₁₊_z₎Sb₂(z=0, 0.02, 0.04)样品存在Mg空位(${{\text{{V}''}}_{\text{Mg}}}$), 表现为p型传导; 而Mg₃₍₁₊_z₎Sb₂ (z=0.06, 0.08)样品中存在间隙Mg($\text{Mg}_{\text{i}}^{\centerdot \centerdot }$), 表现为n型传导。Mg_3(1+0.04)Sb₂样品在较宽温区(室温至770 K)内保持最高的热电优值, 该样品最接近本征p型Mg₃Sb₂化合物的组成和热电性能。本研究表明, Mg含量对Mg₃₍₁₊_z₎Sb₂化合物载流子类型和浓度以及迁移率具有一定的调控作用。

关键词: Mg含量, Mg₃Sb₂化合物, 载流子, 热电性能

Abstract:

Mg₃Sb₂ compound has attracted much attention due to the promising thermoelectric properties and cost advantage. However, it is quite difficult to control Mg content during synthesizing processes because of high saturation vapor pressure and chemical reactivity of Mg element. Herein, Mg₃₍₁₊_z₎Sb₂ (z=0, 0.02, 0.04, 0.06 and 0.08) samples were prepared by combination of solid state reaction, ball milling and spark plasma sintering (SPS). Their effects of Mg content on thermoelectric properties of Mg₃Sb₂ compounds were investigated in this study. Results indicate that actual Mg content rises with nominal Mg content increasing, and their point defect type changes from Mg vacancy(${{\text{{V}''}}_{\text{Mg}}}$) to interstitial Mg($\text{Mg}_{\text{i}}^{\centerdot \centerdot }$), leading to transition of transport behavior from p type (hole carriers predominated) for Mg₃₍₁₊_z₎Sb₂ (z=0, 0.02, 0.04) samples to n type (electron carriers predominated) for Mg₃₍₁₊_z₎Sb₂ (z=0.06, 0.08) samples. Besides, Mg_3(1+0.04)Sb₂ sample shows the highest ZT value from room temperature to 770 K, and achieves maximum ZT of 0.28 at 800 K. Additionally, Mg_3(1+0.04)Sb₂ sample exhibits intrinsic p-type transport behavior for Mg₃Sb₂ compound, which could serve as matrix to be extrinsically doped in the future study for further improvements of electrical properties and ZT value.

Key words: Mg content, Mg₃Sb₂ compound, carriers, thermoelectric property

中图分类号:

O472

逯旭, 侯绩翀, 张强, 樊建锋, 陈少平, 王晓敏. Mg含量对Mg₃₍₁₊_z₎Sb₂化合物热电传输性能的影响[J]. 无机材料学报, 2021, 36(8): 835-840.

LU Xu, HOU Jichong, ZHANG Qiang, FAN Jianfeng, CHEN Shaoping, WANG Xiaomin. Effect of Mg Content on Thermoelectric Property of Mg₃₍₁₊_z₎Sb₂ Compounds[J]. Journal of Inorganic Materials, 2021, 36(8): 835-840.

图/表 5

图1 (a) Mg3(1+z)Sb2(z=0, 0.02, 0.04, 0.06, 0.08)的X射线衍射图谱; Mg3(1+0.04)Sb2样品的(b)抛光表面背散射电子图, (c)Mg元素面分布图和(d)Sb元素面分布图

Fig. 1 (a) XRD patterns of Mg3(1+z)Sb2 (z=0, 0.02, 0.04, 0.06, 0.08), and (b) back scattering electron image and elemental mapping of (c) Mg, (d) Sb for Mg3(1+0.04)Sb2

表1 Mg3(1+z)Sb2(z=0, 0.02, 0.04, 0.06, 0.08)的实际组成

Table 1 Actual compositions of Mg3(1+z)Sb2 (z=0, 0.02, 0.04, 0.06, 0.08)

Nominal composition	Actual composition
Nominal composition	Mg	Sb
Mg₃Sb₂	2.88	2.00
Mg_3.06Sb₂	2.92	2.00
Mg_3.12Sb₂	2.97	2.00
Mg_3.18Sb₂	3.02	2.00
Mg_3.24Sb₂	3.04	2.00

图2 Mg3(1+z)Sb2 (z=0, 0.02, 0.04, 0.06, 0.08)的(a)电导率σ、(b)载流子浓度pH(nH)、(c)霍尔系数RH、(d)迁移率μ、(e)Seebeck系数α和(f)功率因子PF随温度的变化关系曲线

Fig. 2 Temperature dependent electrical transport properties of Mg3(1+z)Sb2 (z=0, 0.02, 0.04, 0.06, 0.08) (a) Electrical conductivity, σ; (b) Carrier concentration, pH(nH); (c) Hall coefficient RH; (d) Mobility, μ; (e) Seebeck coefficient, α; (f) Power factor, PF

图3 Mg3(1+z)Sb2 (z=0, 0.02, 0.04, 0.06, 0.08)的(a)总热导率κ、(b)载流子热导率κC和(c)晶格热导率κL随温度的变化关系

Fig. 3 Temperature dependent thermal conductivities of Mg3(1+z)Sb2 (z=0, 0.02, 0.04, 0.06, 0.08) (a) Total thermal conductivity κ; (b) Carrier thermal conductivity κC; (c) Lattice thermal conductivity κL

图4 Mg3(1+z)Sb2 (z=0, 0.02, 0.04, 0.06, 0.08)的热电优值ZT随温度的变化关系曲线

Fig. 4 Temperature dependent thermoelectric figure of merit ZT of Mg3(1+z)Sb2 (z=0, 0.02, 0.04, 0.06, 0.08)

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Mg含量对Mg₃₍₁₊_z₎Sb₂化合物热电传输性能的影响

Effect of Mg Content on Thermoelectric Property of Mg₃₍₁₊_z₎Sb₂ Compounds

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