Mg2Si0.3Sn0.7掺杂Ag和Li的热电性能对比

袁国才; 陈曦; 黄雨阳; 毛俊西; 禹劲秋; 雷晓波; 张勤勇

doi:10.7498/aps.68.20190247

摘要

采用两步固相法合成了物相均匀的Mg_2(1–x)Ag_2xSi_0.3Sn_0.7 (x = 0, 0.01, 0.02, 0.03, 0.04, 0.05)和Mg_2(1–y)Li_2ySi_0.3Sn_0.7 (y = 0, 0.02, 0.04, 0.06, 0.08)热电材料, 测试了室温物理性能和室温至773 K的热电性能, 研究了不同掺杂剂的固溶度、微观结构、载流子浓度、电性能和热输运. X射线衍射图谱和扫描电子显微镜图像显示掺杂Ag和Li的固溶度分别为x = 0.03和y = 0.06. 根据单抛物线模型, p型的Mg_2(1–x)Ag_2xSi_0.3Sn_0.7和Mg_2(1–y)Li_2ySi_0.3Sn_0.7的有效质量为1.2m₀. 对比结果表明: 掺杂Ag或Li的最大载流子浓度分别达到4.64 × 10¹⁹ cm^–3和15.1 × 10¹⁹ cm^–3; 掺杂Li元素的样品有较高的固溶度、较高的载流子浓度和较高的功率因子PF约为1.62 × 10^–3 W·m^–1·K^–2; 掺杂Li元素样品中较高的载流子浓度能够有效抑制双极效应, 显著降低双极热导率; Mg_1.92Li_0.08Si_0.3Sn_0.7的最大ZT值0.54, 比Mg_1.9Ag_0.1Si_0.3Sn_0.7的最大ZT值0.34提高了大约58%. 根据Callaway理论, 由于质量场波动和应变场波动增强声子散射, 掺杂Ag和Li元素样品的晶格热导率比未掺杂样品明显降低.

关键词:

Abstract

In recent decades, Mg₂(Si, Sn) solid solutions have long been considered as one of the most important classes of eco-friendly thermoelectric materials. The thermoelectric performance of Mg₂(Si, Sn) solid solutions with outstanding characteristics of low-price, non-toxicity, earth-abundant and low-density has been widely studied. The n-type Mg₂(Si, Sn) solid solutions have achieved the dimensionless thermoelectric figure of merit ZT ~1.4 through Bi/Sb doping and convergence of conduction bands. However, the thermoelectric performances for p-type Mg₂(Si, Sn) solid solutions are mainly improved by optimizing the carrier concentration. In this work, the thermoelectric properties for p-type Mg₂Si_0.3Sn_0.7 are investigated and compared with those for different p-type dopant Ag or Li. The homogeneous Mg₂Si_0.3Sn_0.7 with Ag or Li doping is synthesized by two-step solid-state reaction method at temperatures of 873 K and 973 K for 24 h, respectively. The transport parameters and the thermoelectric properties are measured at temperatures ranging from room temperature to 773 K for Mg_2(1–x)Ag_2xSi_0.3Sn_0.7 (x = 0, 0.01, 0.02, 0.03, 0.04, 0.05) and Mg_2(1–y)Li_2ySi_0.3Sn_0.7 (y = 0, 0.02, 0.04, 0.06, 0.08) samples. The influences of different dopants on solid solubility, microstructure, carrier concentration, electrical properties and thermal transport are also investigated. The X-ray diffraction (XRD) patterns and scanning electron microscopy (SEM) images show that the solid solubility for Ag and for Li are x = 0.03 and y = 0.06, respectively. Based on the assumption of single parabolic band model, the value of effective mass ~1.2m₀ of p-type Mg_2(1–x)Ag_2xSi_0.3Sn_0.7 and Mg_2(1–y)Li_2ySi_0.3Sn_0.7 are similar to that reported in the literature. The comparative results demonstrate that the maximum carrier concentration for Ag doping and for Li doping are 4.64×10¹⁹ cm^–3 for x = 0.01 and 15.1×10¹⁹ cm^–3 for y = 0.08 at room temperature, respectively; the Li element has higher solid solubility in Mg₂(Si, Sn), which leads to higher carrier concentration and power factor PF ~1.62×10^–3 ${\rm W}\cdot{\rm m^{–1}}\cdot{\rm K^{–2}}$ in Li doped samples; the higher carrier concentration of Li doped samples effectively suppresses the bipolar effect; the maximum of ZT ~0.54 for Mg_1.92Li_0.08Si_0.3Sn_0.7 is 58% higher than that of Mg_1.9Ag_0.1Si_0.3Sn_0.7 samples. The lattice thermal conductivity of Li or Ag doped sample decreases obviously due to the stronger mass and strain field fluctuations in phonon transport.

Keywords:

作者及机构信息

1.
西华大学材料科学与工程学院, 成都　610039

2.
西华大学西华学院, 成都　610039

通信作者: 张勤勇, zhangqy@mail.xhu.edu.cn

基金项目: 国家自然科学基金(批准号: 51572226)、四川省科技支撑计划(批准号: 2015GZ0060)和国家创新创业训练项目(批准号: 201710623)资助的课题.

Authors and contacts

1.
School of Materials Science and Engineering, Xihua University, Chengdu 610039, China

2.
Xihua Honor College, Xihua University, Chengdu 610039, China

Corresponding author: Zhang Qin-Yong, zhangqy@mail.xhu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 51572226), the Science and Technology Foundation of Sichuan Province, China (Grant No. 2015GZ0060), and the Chinese Innovation and Entrepreneurship Training Project (Grant No. 201710623).

文章全文 : translate this paragraph

参考文献

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施引文献

图 1 Mg_2(1－x)Ag_2xSi_0.3Sn_0.7(0 ≤ x ≤ 0.05)和Mg_2(1－y)Li_2ySi_0.3Sn_0.7(0 ≤ y ≤ 0.08)的XRD图谱(a), (c)与晶格常数(b), (d)

Fig. 1. XRD patterns (a), (c) and lattice constant (b), (d) of Mg_2(1－x)Ag_2xSi_0.3Sn_0.7 (0 ≤ x ≤ 0.05) and Mg_2(1－y)Li_2ySi_0.3Sn_0.7 (0 ≤ y ≤ 0.08)

下载: 全尺寸图片幻灯片

图 2 (a), (b), (c)分别为Mg₂Si_0.3Sn_0.7, Mg_1.9Ag_0.1Si_0.3Sn_0.7，Mg_1.92Li_0.08Si_0.3Sn_0.7的SEM图像; (d) Mg_1.92Li_0.08Si_0.3Sn_0.7的背散射图像

Fig. 2. (a), (b) and (c) are SEM images of Mg₂Si_0.3Sn_0.7, Mg_1.9Ag_0.1Si_0.3Sn_0.7, and Mg_1.92Li_0.08Si_0.3Sn_0.7; (d) the back scattered electron image of Mg_1.92Li_0.08Si_0.3Sn_0.7

下载: 全尺寸图片幻灯片

图 3 Seebeck系数S与载流子浓度p之间的Pisarenko关系

Fig. 3. The Pisarenko plot between Seebeck coefficient S and carrier concentration p

下载: 全尺寸图片幻灯片

图 4 (a)—(f) Mg_2(1－x)Ag_2xSi_0.3Sn_0.7(0 ≤ x ≤ 0.05)和Mg_2(1－y)Li_2ySi_0.3Sn_0.7(0 ≤ y ≤ 0.08)的电导率、Seebeck系数和功率因子与温度的关系

Fig. 4. The temperature dependence of (a), (d) electrical conductivity, (b), (e) Seebeck coefficient and (c), (f) power factor for Mg_2(1－x)Ag_2xSi_0.3Sn_0.7 (0 ≤ x ≤ 0.05) and Mg_2(1－y)Li_2ySi_0.3Sn_0.7 (0 ≤ y ≤ 0.08)

下载: 全尺寸图片幻灯片

图 5 (a)—(f) Mg_2(1－x)Ag_2xSi_0.3Sn_0.7(0 ≤ x ≤ 0.05)和Mg_2(1－y)Li_2ySi_0.3Sn_0.7(0 ≤ y ≤ 0.08)的热导率, 晶格热导率和ZT值与温度的关系图

Fig. 5. The temperature dependence of (a), (d) thermal conductivity, (b), (e) lattice thermal conductivity and (c), (f) ZT for Mg_2(1－x)Ag_2xSi_0.3Sn_0.7(0 ≤ x ≤ 0.05) and Mg_2(1－y)Li_2ySi_0.3Sn_0.7(0 ≤ y ≤ 0.08)

下载: 全尺寸图片幻灯片

图 6 Mg₂Si_0.3Sn_0.7的掺杂Ag和Li浓度与质量场波动散射因子Γ_M和应变场波动散射因子Γ_S的关系

Fig. 6. The relation of (a) the mass fluctuation scattering parameter Γ_M, (b) strain field fluctuation scattering parameter Γ_S and doping Ag, Li content of Mg₂Si_0.3Sn_0.7

下载: 全尺寸图片幻灯片

表 1 Mg_2(1－x)Ag_2xSi_0.3Sn_0.7(0 ≤ x ≤ 0.05)和Mg_2(1－y)Li_2ySi_0.3Sn_0.7(0 ≤ y ≤ 0.08)在300 K的物理参数

Table 1. Physical parameters of Mg_2(1－x)Ag_2xSi_0.3Sn_0.7 (0 ≤ x ≤ 0.05) and Mg_2(1－y)Li_2ySi_0.3Sn_0.7 (0 ≤ y ≤ 0.08) at 300 K

Composition	σ/10⁴ S·m^–1	R_H/cm³·C^–1	p/10¹⁹ cm^–3	μ/cm²·V^–1·s^–1	S/μV·K^–1	m^*(m₀)
x = 0	0.15	–3.22	–0.19	48.3	–458.0	1.6
x = 0.01	3.48	0.135	4.64	46.8	154.7	1.2
x = 0.02	3.33	0.173	3.60	57.7	166.4	1.1
x = 0.03	3.73	0.186	3.35	69.5	163.8	1.0
x = 0.04	3.11	0.155	4.03	48.2	160.6	1.1
x = 0.05	3.62	0.153	4.09	53.7	154.7	1.1
y = 0.02	11.20	0.056	11.10	63.1	90.7	1.0
y = 0.04	9.65	0.044	14.00	42.8	91.3	1.2
y = 0.06	13.14	0.042	14.70	55.8	82.2	1.1
y = 0.08	9.74	0.041	15.10	40.2	83.9	1.2

下载: 导出CSV

[1]	Dresselhaus M S, Chen G, Tang M Y, Yang R G, Lee H, Wang D Z, Ren Z F, Fleurial J P, Gogna P 2007 Adv. Mater. 19 1043 Google Scholar
[2]	Snyder G J, Toberer E S 2008 Nat. Mater. 7 105 Google Scholar
[3]	Bell L E 2008 Science 321 1457 Google Scholar
[4]	Zhu T, Liu Y, Fu C, Heremans J P, Snyder G J, Zhao X 2017 Adv. Mater. 29 1605884 Google Scholar
[5]	朱航天, 任武洋, 张勤勇, 任志锋 2018 西华大学学报(自然科学版) 37 15 Google Scholar Zhu H T, Ren W Y, Zhang Q Y, Ren Z F 2018 J. Xihua Univ. (Natural Science Edition) 37 15 Google Scholar
[6]	Pei Y, Shi X, Lalonde A, Wang H, Chen L, Snyder G J 2011 Nature 473 66 Google Scholar
[7]	Mao J, Wang Y, Ge B, Jie Q, Liu Z, Saparamadu U, Liu W, Ren Z 2016 Phys. Chem. Chem. Phys. 18 20726 Google Scholar
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[9]	Pei Y, Lalonde A D, Wang H, Snyder G J 2012 Energy Environ. Sci. 5 7963 Google Scholar
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[11]	Paul B, Ajay Kumar V, Banerji P 2010 J. Appl. Phys. 108 064322 Google Scholar
[12]	Xie W J, Yan Y G, Zhu S, Zhou M, Populoh S, Gałązka K, Poon S J, Weidenkaff A, He J, Tang X F, Tritt T M 2013 Acta Mater. 61 2087 Google Scholar
[13]	Heremans J P, Wiendlocha B, Chamoire A M 2012 Energy Environ. Sci. 5 5510 Google Scholar
[14]	Zhang Q, Wang H, Liu W, Wang H, Yu B, Zhang Q, Tian Z, Ni G, Lee S, Esfarjani K, Chen G, Ren Z 2012 Energy Environ. Sci. 5 5246 Google Scholar
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[16]	Xiao Y, Wu H, Li W, Yin M, Pei Y, Zhang Y, Fu L, Chen Y, Pennycook S J, Huang L, He J, Zhao L D 2017 J. Am. Chem. Soc. 139 18732 Google Scholar
[17]	王浚臣, 袁国才, 禹劲秋, 莫小波, 金应荣, 黄丽宏 2018 西华大学学报(自然科学版) 37 68 Google Scholar Wang J C, Yuan G C, Yu J Q, Mo X B, Jin Y R, Huang L H 2018 Journal of Xihua University (Natural Science Edition) 37 68 Google Scholar
[18]	de Boor J, Dasgupta T, Saparamadu U, Müller E, Ren Z F 2017 Mater. Today Energy 4 105 Google Scholar
[19]	Bashir M B A, Mohd Said S, Sabri M F M, Shnawah D A, Elsheikh M H 2014 Renewable and Sustainable Energy Reviews 37 569 Google Scholar
[20]	Santos R, Aminorroaya Yamini S, Dou S X 2018 J. Mater. Chem. A 6 3328 Google Scholar
[21]	Liu W, Yin K, Zhang Q, Uher C, Tang X 2017 Nat. Sci. Rev. 4 611 Google Scholar
[22]	Pulikkotil J J, Singh D J, Auluck S, Saravanan M, Misra D K, Dhar A, Budhani R C 2012 Phys. Rev. B 86 155204 Google Scholar
[23]	Sun J, Singh D J 2016 Phys. Rev. Appl. 5 024006 Google Scholar
[24]	Tani J I, Kido H 2008 Intermetallics 16 418 Google Scholar
[25]	Tani J I, Kido H 2012 Physica B 407 3493 Google Scholar
[26]	Imai Y, Mori Y, Nakamura S, Takarabe K I 2013 J. Alloys Compd. 549 175 Google Scholar
[27]	Tani J I, Kido H 2008 J. Alloys Compd. 466 335 Google Scholar
[28]	Zhang Q, He J, Zhao X B, Zhang S N, Zhu T J, Yin H, Tritt T M 2008 J. Phys. D: Appl. Phys. 41 185103 Google Scholar
[29]	Luo W J, Yang M J, Fei C, Shen Q, Jiang H G, Zhang L M 2010 Mater. Trans. 51 288 Google Scholar
[30]	Liu W, Tang X, Li H, Yin K, Sharp J, Zhou X, Uher C 2012 J. Mater. Chem. 22 13653 Google Scholar
[31]	Ihou-Mouko H, Mercier C, Tobola J, Pont G, Scherrer H 2011 J. Alloys Compd. 509 6503 Google Scholar
[32]	Tada S, Isoda Y, Udono H, Fujiu H, Kumagai S, Shinohara Y 2014 J. Electron. Mater. 43 1580
[33]	Zhang Q, Cheng L, Liu W, Zheng Y, Su X, Chi H, Liu H, Yan Y, Tang X, Uher C 2014 Phys. Chem. Chem. Phys. 16 23576 Google Scholar
[34]	Tang X, Zhang Y, Zheng Y, Peng K, Huang T, Lu X, Wang G, Wang S, Zhou X 2017 Appl. Therm. Eng. 111 1396 Google Scholar
[35]	Yin K, Zhang Q, Zheng Y, Su X, Tang X, Uher C 2015 J. Mater. Chem. C 3 10381 Google Scholar
[36]	Liu W, Chi H, Sun H, Zhang Q, Yin K, Tang X, Zhang Q, Uher C 2014 Phys. Chem. Chem. Phys. 16 6893 Google Scholar
[37]	de Boor J, Saparamadu U, Mao J, Dahal K, Müller E, Ren Z 2016 Acta Mater. 120 273 Google Scholar
[38]	Saparamadu U, de Boor J, Mao J, Song S, Tian F, Liu W, Zhang Q, Ren Z 2017 Acta Mater. 141 154 Google Scholar
[39]	Gao P, Davis J D, Poltavets V V, Hogan T P 2016 J. Mater. Chem. C 4 929 Google Scholar
[40]	Tang X, Wang G, Zheng Y, Zhang Y, Peng K, Guo L, Wang S, Zeng M, Dai J, Wang G, Zhou X 2016 Scripta Mater. 115 52 Google Scholar
[41]	Kim H S, Gibbs Z M, Tang Y, Wang H, Snyder G J 2015 APL Mater. 3 041506 Google Scholar
[42]	Yang J, Meisner G P, Chen L 2004 Appl. Phys. Lett. 85 1140 Google Scholar
[43]	覃玉婷, 仇鹏飞, 史迅, 陈立东 2017 无机材料学报 32 1171 Qin Y T, Qiu P F, Shi X, Chen L D 2017 J. Inorg. Mater. 32 1171
[44]	Slack G A 1957 Phys. Rev. 105 832 Google Scholar
[45]	Abeles B 1963 Phys. Rev. 131 1906 Google Scholar

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Mg₂Si_0.3Sn_0.7掺杂Ag和Li的热电性能对比

Comparative study of thermoelectric properties of Mg₂Si_0.3Sn_0.7 doped by Ag or Li

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Abstract

作者及机构信息

1.
西华大学材料科学与工程学院, 成都　610039

2.
西华大学西华学院, 成都　610039

通信作者: 张勤勇, zhangqy@mail.xhu.edu.cn

Authors and contacts

1.
School of Materials Science and Engineering, Xihua University, Chengdu 610039, China

2.
Xihua Honor College, Xihua University, Chengdu 610039, China

Corresponding author: Zhang Qin-Yong, zhangqy@mail.xhu.edu.cn

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