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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 Mg3.275Mn0.025Sb1.49Bi0.5Te0.01/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.
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Keywords:
- nano-SiO2 /
- Mg3Sb2-based materials /
- composite /
- thermoelectric transport properties
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Google Scholar
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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
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[7] Imasato K, Kang S D, Snyder G J 2019 Energy Environ. Sci. 12 965
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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
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Google Scholar
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Google Scholar
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Google Scholar
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Google Scholar
[19] Imasato K, Wood M, Anand S, Kuo J J, Snyder G J 2022 Adv. Energy Sustainability Res. 3 2100208
Google Scholar
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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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图 1 不同SiO2含量的Mg3.275Mn0.025Sb1.49Bi0.5Te0.01 XRD图谱
Figure 1. XRD of Mg3.275Mn0.025Sb1.49Bi0.5Te0.01 with different SiO2 content.
图 2 (a), (b), (d)不同SiO2含量的Mg3.275Mn0.025Sb1.49Bi0.5Te0.01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
Figure 2. (a), (b) and (d) are temperature dependence curves of electrical properties of Mg3.275Mn0.025Sb1.49Bi0.5Te0.01 with different SiO2 content; (c) change trend of reduced Fermi level of samples at room temperature and 723 K.
图 3 室温霍尔载流子浓度与迁移率随SiO2含量变化关系图
Figure 3. The composition dependence of hall carrier concentration and mobility at room temperature.
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
Figure 4. Relation curve of Seebeck coefficient and power factor as conductivity function at 723 K.
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
Figure 5. Temperature dependence curve of thermal diffusivity (a) and thermal conductivity (b).
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
Figure 6. The temperature dependence curves of Lorentz constant (a), electronic thermal conductivity (b), electronic thermal conductivity ratio (c) and lattice thermal conductivity (d).
图 7 不同纳米SiO2含量的Mg3.3Sb1.5Bi0.49Te0.01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
Figure 7. Temperature dependence curve of ZT value of Mg3.3Sb1.5Bi0.49Te0.01 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.
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[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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