Enhanced Thermoelectric Performance of P-Doped Silicon-Germanium Alloys Synthesized by High-Pressure Method
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摘要: 热电材料是一种可以实现热能与电能相互转换的功能材料，硅锗合金作为优良的高温热电材料被应用于深空探测。采用高压合成法制备了磷掺杂n型SiGe合金Si80Ge20Px （x=0, 1, 2），研究了其电输运和热输运特性。结果表明，高压合成样品具有多尺度缺陷。磷掺杂可以优化SiGe合金的电导率和Seebeck系数，1050 K时Si80Ge20P1样品的功率因子较未掺杂样品提升了100%。同时，掺磷量的增加导致晶格热导率下降，1050 K时Si80Ge20P2样品的热导率降低约80%。此外，Si80Ge20Px的热电性能得到显著提升，1050 K时Si80Ge20P2样品的热电优值达到1.1。Abstract: Thermoelectric material is a kind of functional material which could realize the conversion between thermal energy and electric energy. Silicon-germanium (SiGe) alloy is used in deep space exploration as a kind of high temperature thermoelectric material. In this work, P-doped n-type SiGe alloy was prepared by high pressure synthesis method. The electrical and thermal transport properties of Si80Ge20Px (x=0, 1, 2) were characterized. The results show that the samples synthesized under high pressure have multi-scale defects. P-doping could optimize the electrical conductivity and Seebeck coefficient of SiGe alloy, the power factor of Si80Ge20P1 sample is 100% higher than that of the undoped sample at 1050 K. Furthermore, the increase of P content leads to the decrease of lattice thermal conductivity, and the thermal conductivity of Si80Ge20P2 sample decreases by about 80% at 1050 K. The thermoelectric properties of SiGe alloy are significantly improved, and the maximum figure of merit of Si80Ge20P2 sample reached 1.1 at 1050 K.
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图 1 国产六面顶压机(a)、碳化钨顶砧(b)和高压合成SiGe合金组装(c)
Figure 1. Domestic cubic high-pressure equipment (a), tungsten carbide anvil (b), and assembly of SiGe alloy synthesized by high-pressure (c)
图 2 SiGe样品的XRD谱：(a) 混合球磨4 h的Si80Ge20P2原料粉末；(b)～(d) 高压合成的Si80Ge20Px (x=0, 1, 2)合金
Figure 2. XRD patterns of SiGe samples: (a) Si80Ge20P2 raw materials mixed by ball milling for 4 h; (b) – (d) Si80Ge20Px (x=0, 1, 2) alloys synthesized by high-pressure method
图 3 高压合成的Si80Ge20P1显微图像：(a) SEM图像，(b) HR-TEM图像
Figure 3. SEM (a) and HR-TEM (b) images of Si80Ge20P1 alloys synthesized by high-pressure method
图 4 Si80Ge20Px （x=0, 1, 2）的电导率(a)、Seebeck系数(b)、功率因子(c)与温度的关系
Figure 4. Temperature dependence of (a) electrical conductivity, (b) Seebeck coefficient, and (c) power factor of Si80Ge20Px (x=0, 1, 2) alloys
图 5 Si80Ge20Px（x=0, 1, 2）合金的热导率(a)与晶格热导率(b)与温度的关系
Figure 5. Temperature dependence of (a) thermal conductivity and (b) lattice thermal conductivity of Si80Ge20Px (x=0, 1, 2) alloys
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