纳米SiO2复合对Mg3Sb2基材料热电性能的影响

高君玲; 赵怀周; 许艳丽

doi:10.7498/aps.72.20230176

摘要

Mg₃(Sb, Bi)₂基热电材料由于其优异的热电性能和较低的成本近来受到广泛的关注. 本研究通过将纳米SiO₂复合进成分为Mg_3.275Mn_0.025Sb_1.49Bi_0.5Te_0.01的基体相中, 考察其热电输运性能的变化及机制. 结果表明, 当SiO₂复合进Mg₃Sb₂基材料中时, 由于引进大量的微小晶界, 能有效地散射声子, 促使晶格热导率降低, 优化热输运性能, 如SiO₂体积含量为0.54%时, 室温时热导率由复合前的1.24 W/(m·K)降至1.04 W/(m·K), 降幅达到15%; 同时其对电子也产生强烈的散射作用, 导致迁移率和电导率大幅下滑, 结果表现为近室温区功率因子剧烈衰减, 恶化了电输运性能. 电性能相对于热性能较大降低幅度使得材料在整个测试温区的热电优值没有得到改善. 纳米SiO₂作为Mg₃Sb₂基热电材料复合物来调控热电性能是有效的备选物质, 可结合其他手段改善输运特性, 如在晶界处适当修饰, 降低载流子传输的晶界势垒, 能够提升该体系的综合热电性能.

关键词:

Abstract

Recently, Mg₃(Sb,Bi)₂-based thermoelectric materials have received extensive attention owing to excellent thermoelectric properties and the low cost. This study investigates the change and mechanism of thermoelectric transport properties of Mg_3.275Mn_0.025Sb_1.49Bi_0.5Te_0.01/SiO₂ nanocomposite. The results show that nano-SiO₂ can effectively scatter phonons, promote the reduction of lattice thermal conductivity, and optimize the heat transport performance owing to the introduction of a large number of tiny grain boundaries. For example, when SiO₂ content is 0.54%, the thermal conductivity decreases by 15% from 1.24 W/(m·K) to 1.04 W/(m·K) compared with that of 0% SiO₂ sample at room temperature. At the same time, the material system also has a strong scattering effect on electrons. This leads to a sharp attenuation of power factor and electrical transport performance with decline of mobility and conductivity in the room temperature area. Nano SiO₂ is an effective candidate for regulating thermoelectric properties of Mg₃Sb₂ based thermoelectric material. The thermoelectric transport performance of the material will be improved by combining with other methods, such as appropriate grain boundary modification to reduce the potential barrier of charge carrier transport.

Keywords:

作者及机构信息

1.
长治学院物理系, 长治　046011

2.
中国科学院物理研究所, 北京凝聚态物理国家实验室, 北京　100190

通信作者: 高君玲, calm228@163.com

基金项目: 山西省高等学校科技创新计划(批准号: 2021L511)资助的课题.

Authors and contacts

1.
Department of Physics, Changzhi University, Changzhi 046011, China

2.
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China

Corresponding author: Gao Jun-Ling, calm228@163.com

Funds: Project supported by the Scientific and Technological Innovation Programs of Higher Education Institutions of Shanxi Province, China (Grant No. 2021L511).

文章全文 : translate this paragraph

参考文献

[1]	Mao J, Liu Z, Zhou J, Zhu H, Zhang Q, Chen G, Ren Z 2018 Adv. Phys. 67 69 Google Scholar
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施引文献

图 1 不同SiO₂含量的Mg_3.275Mn_0.025Sb_1.49Bi_0.5Te_0.01XRD图谱

Fig. 1. XRD of Mg_3.275Mn_0.025Sb_1.49Bi_0.5Te_0.01 with different SiO₂content.

下载: 全尺寸图片幻灯片

图 2 (a), (b), (d)不同SiO₂含量的Mg_3.275Mn_0.025Sb_1.49Bi_0.5Te_0.01电性能温度依赖曲线; (c)室温和723 K时样品的简约费米能级变化趋势图

Fig. 2. (a), (b) and (d) are temperature dependence curves of electrical properties of Mg_3.275Mn_0.025Sb_1.49Bi_0.5Te_0.01 with different SiO₂ content; (c) change trend of reduced Fermi level of samples at room temperature and 723 K.

下载: 全尺寸图片幻灯片

图 3 室温霍尔载流子浓度与迁移率随SiO₂含量变化关系图

Fig. 3. The composition dependence of hall carrier concentration and mobility at room temperature.

下载: 全尺寸图片幻灯片

图 4 塞贝克系数、功率因子作为电导率函数在723 K时的关系曲线

Fig. 4. Relation curve of Seebeck coefficient and power factor as conductivity function at 723 K.

下载: 全尺寸图片幻灯片

图 5 实验测试的热扩散系数(a)和热导率(b)的温度依赖关系曲线

Fig. 5. Temperature dependence curve of thermal diffusivity (a) and thermal conductivity (b).

下载: 全尺寸图片幻灯片

图 6 计算所得洛伦兹常数(a)、电子热导率(b)、电子热导率占比(c)和晶格热导率(d)的温度依赖关系曲线

Fig. 6. The temperature dependence curves of Lorentz constant (a), electronic thermal conductivity (b), electronic thermal conductivity ratio (c) and lattice thermal conductivity (d).

下载: 全尺寸图片幻灯片

图 7 不同纳米SiO₂含量的Mg_3.3Sb_1.5Bi_0.49Te_0.01样品ZT值温度依赖曲线; 插图为纳米SiO₂复合的Mg₃Sb₂基材料样品电子和声子输运过程中的散射原理图

Fig. 7. Temperature dependence curve of ZT value of Mg_3.3Sb_1.5Bi_0.49Te_0.01 samples with different nano-SiO₂ content; the illustration shows the scattering schematic diagram of the electron and phonon transport process of the composite with Mg₃Sb₂-based material and nano-SiO₂.

下载: 全尺寸图片幻灯片

[1]	Mao J, Liu Z, Zhou J, Zhu H, Zhang Q, Chen G, Ren Z 2018 Adv. Phys. 67 69 Google Scholar
[2]	Kim S I, Lee K H, Mun H A, Kim H S, Hwang S W, Roh J W, Yang D J, Shin W H, Li X S, Lee Y H 2015 Science 348 109 Google Scholar
[3]	Pei Y, Shi X, LaLonde A, Wang H, Chen L, Snyder G J 2011 Nature 473 66 Google Scholar
[4]	He J, Tritt T M 2017 Science 357 eaak9997 Google Scholar
[5]	Boona S R, Myers R C, Heremans J P 2014 Energy Environ. Sci. 7 885 Google Scholar
[6]	Zheng Y, Lu T, Polash M M, Rasoulianboroujeni M, Liu N, Manley M E, Deng Y, Sun P, Chen X, Hermann R P, Vashaee D, Heremans J P, Zhao H 2019 Sci. Adv. 5 eaat9461 Google Scholar
[7]	Imasato K, Kang S D, Snyder G J 2019 Energy Environ. Sci. 12 965 Google Scholar
[8]	Ren Z, Shuai J, Mao J, Zhu Q, Song S, Ni Y, Chen S 2018 Acta Mater. 143 265 Google Scholar
[9]	Imasato K, Kang S D, Ohno S, Snyder G J 2018 Mater. Horiz. 5 59 Google Scholar
[10]	Tamaki H, Sato H K, Kanno T 2016 Adv. Mater. 28 10182 Google Scholar
[11]	Shuai J, Ge B, Mao J, Song S, Wang Y, Ren Z 2018 J. Am. Chem. Soc. 140 1910 Google Scholar
[12]	Imasato K, Ohno S, Kang S D, Snyder G J 2018 APL Mater. 6 016106 Google Scholar
[13]	Wood M, Kuo J J, Imasato K, Snyder G J 2019 Adv. Mater. 31 1902337 Google Scholar
[14]	Mao J, Zhu H, Ding Z, Liu Z, Gamage G A, Chen G, Ren Z 2019 Science 365 495
[15]	Yang J, Li G, Zhu H, Chen N, Lu T, Gao J, Guo L, Xiang J, Sun P, Yao Y 2022 Joule 6 193 Google Scholar
[16]	Ren P, Liu Y, He J, Lv T, Gao J, Xu G 2018 Inorg. Chem. Front. 5 2380 Google Scholar
[17]	Shi X, Wang X, Li W, Pei Y 2018 Small Methods 2 1800022 Google Scholar
[18]	Brod M K, Anand S, Snyder G J 2023 Mater. Today Phys. 31 100959 Google Scholar
[19]	Imasato K, Wood M, Anand S, Kuo J J, Snyder G J 2022 Adv. Energy Sustainability Res. 3 2100208 Google Scholar
[20]	Sharp J W, Volckmann E H, Goldsmid H J 2001 Phys. Status Solidi A 185 257 Google Scholar
[21]	Sharp J W, Goldsmid H J 1999 Proceedings of the 18th International Conference on Thermoelectrics Baltimore, USA, August 29–September 2, 1999 p709
[22]	Jin H, Heremans J P 2018 Phys. Rev. Mater. 2 115401 Google Scholar
[23]	Kuo J J, Kang S D, Imasato K, Tamaki H, Ohno S, Kanno T, Snyder G J 2018 Energy Environ. Sci. 11 429 Google Scholar
[24]	Kanno T, Tamaki H, Sato H K, Kang S D, Ohno S, Imasato K, Kuo J J, Snyder G J, Miyazaki Y 2018 Appl. Phys. Lett. 112 033903 Google Scholar
[25]	Mao T, Qiu P, Liu J, Du X, Hu P, Zhao K, Ren D, Shi X, Chen L 2020 Phys. Chem. Chem. Phys. 22 7374 Google Scholar

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纳米SiO₂复合对Mg₃Sb₂基材料热电性能的影响