AgSn18SbTe20无铅中温热电材料的粉末冶金法制备工艺及其对性能的影响

doi:10.15541/jim20140501

摘要/Abstract

摘要：

研究了制备p型AgSn₁₈SbTe₂₀无铅热电材料的机械合金化(MA)结合放电等离子烧结(SPS)工艺, 调查了MA过程中球磨时间和SPS温度对材料电热传输性能和热电优值的影响, 分析了样品的物相和显微结构。研究表明, 适当延长球磨时间和降低烧结温度, 可以有效提高材料的热电性能。优化制备条件可以实现59%的性能提升, 最佳条件(球磨12 h、SPS温度743 K)下制备的样品ZT值在723 K达到0.62。

关键词: 热电材料, 机械合金化, 放电等离子烧结, AgSn18SbTe20

Abstract:

Lead-free thermoelectric materials gain increasing attention for environmentally friendly power- generation applications derived from waste-heat sources. In this work, mid-temperature lead-free p-type AgSn₁₈SbTe₂₀ thermoelectric materials were fabricated by a process combining mechanical alloying (MA) and spark plasma sintering (SPS). Electrical conductivity, Seeback coefficient, power factor and thermal conductivity of the sintered samples were measured in the temperature range from 300 K to 723 K, and the thermoelectric figure of merit, ZT, values were calculated. The phase structures and morphologies of the samples were observed. The effects of milling time and sintering temperatures on thermoelectric properties were investigated. And the results show that properly prolonging milling time and decreasing sintering temperature can enhance thermoelectric performance of the materials. The ZT value can be enhanced by 59% through optimizing the processing parameters, resulting in a relatively high ZT up to 0.62 at 723 K when the materials are milled for 12 h and sintered at 743 K.

Key words: thermoelectric materials, mechanical alloying, spark plasma sintering, AgSn18SbTe20

中图分类号:

TB34

邢志波, 李敬锋. AgSn₁₈SbTe₂₀无铅中温热电材料的粉末冶金法制备工艺及其对性能的影响[J]. 无机材料学报, 2015, 30(8): 872-876.

XING Zhi-Bo, LI Jing-Feng. Powder Metallurgic Synthesis of Mid-temperature Lead-free AgSn₁₈SbTe₂₀ Thermoelectric Materials and Processing Influence on Thermoelectric Performance[J]. Journal of Inorganic Materials, 2015, 30(8): 872-876.

图/表 8

图1 不同球磨时间的粉体样品和不同温度SPS烧结得到块体样品断面的XRD图谱

Fig. 1 XRD patterns of powders milled for different time and bulk samples SPS sintered at different temperatures

图2 不同球磨时间的粉体样品和不同温度SPS烧结得到的块体样品断面SEM照片

Fig. 2 SEM images of powders milled for different time and bulks sintered at different temperatures after milled for 12 h (a) 4 h; (b) 8 h; (c) 12 h; (d) 12 h-803 K; (e) 12 h-773 K; (f) 12 h-743 K

表1 不同球磨时间743K烧结和球磨12h不同温度烧结得到的块体样品的密度

Table 1 Density carrier concentrationcarrier concentrationcarrier concentrationcarrier concentrationcarrier concentrationof bulks sintered at 743 K with different milling times and of bulks sintered at different temperatures milled for 12 h

Milling time/h	4	8	12	16
Density/ (g·cm^-3)	6.15	6.19	6.17	6.21
Sintering temperature/K	743	773	803
Density/ (g·cm^-3)	6.17	6.21	6.28

图3 不同球磨时间(a)和不同烧结温度(b)得到块体样品的电导率随测试温度变化曲线图

Fig. 3 Temperature dependence of the electrical conductivities carrier concentrationcarrier concentrationcarrier concentrationcarrier concentrationcarrier concentrationof bulks sintered at 803 K with different milling time (a) and sintered at different temperatures after milled for 12 h (b)

图4 不同球磨时间(a)和不同烧结温度(b)得到块体样品的赛贝克系数随测试温度变化曲线图

Fig. 4 Temperature dependence of the Seebeck coefﬁcient of bulks sintered at 803 K with different milling time (a) and sintered at different temperatures after milled for 12 h (b)

图5 不同球磨时间(a)和不同烧结温度(b)得到块体样品的功率因子随温度变化曲线图

Fig. 5 Temperature dependence of the power factor of bulks sintered at 803 K with different milling time (a) and sintered at different temperatures after milled at 12 h (b)

图6 不同球磨时间(a)和不同烧结温度(b)块体样品的热导率随测试温度变化曲线图

Fig. 6 Temperature dependence of the thermal conductivity of bulks sintered with different milling time (a) and different temperatures (b)

图7 不同球磨时间(a)和不同温度烧结(b)得到块体样品的热电优值ZT随测试温度变化曲线图

Fig. 7 Temperature dependence of ZT value of bulks sintered at 803 K with different milling time (a) and sintered at different temperatures after milled for 12 h (b)

参考文献 13

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AgSn₁₈SbTe₂₀无铅中温热电材料的粉末冶金法制备工艺及其对性能的影响

Powder Metallurgic Synthesis of Mid-temperature Lead-free AgSn₁₈SbTe₂₀ Thermoelectric Materials and Processing Influence on Thermoelectric Performance

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