P型Si80Ge20B0.6-SiC纳米复合材料的微观结构与热电性能研究

doi:10.15541/jim20160060

摘要/Abstract

摘要：

采用感应熔炼、球磨与放电等离子烧结的方法制备了SiC第二相均匀分布的Si₈₀Ge₂₀B_0.6-SiC纳米复合热电材料。系统研究了细化Si₈₀Ge₂₀B_0.6晶粒尺寸与复合SiC纳米颗粒对材料热电性能的影响。球磨导致的Si₈₀Ge₂₀B_0.6晶粒尺寸的降低显著增加了材料的晶界数量, 进而增强了晶界对中长波声子的散射, 能够有效降低材料的晶格热导。Si₈₀Ge₂₀B_0.6基体中均匀分布的纳米SiC颗粒提供了额外的散射中心和界面,可进一步增强声子散射,降低材料的晶格热导。在纳米结构化与SiC纳米复合的共同作用下, 材料在1000 K 时热电优值ZT达到了0.62, 较基体提高了17%。证明纳米结构化与纳米复合方法能够共同作用于硅锗合金, 提高其热电性能。

关键词: 硅锗合金, SiC纳米颗粒, 热电材料, 纳米复合, 纳米结构

Abstract:

P-type silicon germanium (SiGe) alloys, Si₈₀Ge₂₀B_0.6, with homogeneously dispersed SiC nanoparticles were prepared by ball milling and subsequent spark plasma sintering. The influence of grain size reduction of SiGe matrix and SiC nanoparticle dispersion on electrical and thermal transport properties were investigated. A significant reduction in lattice thermal conductivity is achieved by a more pronounced grain boundary scattering of phonons introduced by grain size reduction after ball milling. Dispersing SiC nanoparticles in the Si₈₀Ge₂₀B_0.6 matrix effectively reduces the conduction of heat by providing additional phonon scattering centers. A dimensionless figure-of-merit (ZT) of 0.62 at 1000 K is obtained in nanostructuring Si₈₀Ge₂₀B_0.6 incorporated with only 0.5vol% SiC nanoparticles, which is 17% higher than the parent Si₈₀Ge₂₀B_0.6 matrix and about 30% higher than p-type SiGe alloy used in the radioisotope thermoelectric generator in space missions.

Key words: SiGe alloys, SiC nanoparticle dispersion, thermoelectric material, nanocomposite, nanostructuring

中图分类号:

TQ174

杨小燕, 吴洁华, 任都迪, 张天松, 陈立东. P型Si₈₀Ge₂₀B_0.6-SiC纳米复合材料的微观结构与热电性能研究[J]. 无机材料学报, 2016, 31(9): 997-1003.

YANG Xiao-Yan, WU Jie-Hua, REN Du-Di, ZHANG Tian-Song, CHEN Li-Dong. Microstructure and Thermoelectric Properties of p-type Si₈₀Ge₂₀B_0.6-SiC Nanocomposite[J]. Journal of Inorganic Materials, 2016, 31(9): 997-1003.

图/表 8

Fig. 1 Powder XRD patterns of Si80Ge20B0.6 matrix, Si80Ge20B0.6 BM and Si80Ge20B0.6 + 0.5vol% SiC BM samples before SPS. The inset in the upper right depicts XRD pattern of Si80Ge20B0.6 + 0.5vol% SiC BM sample sintered by SPS

Fig. 2 SEM images of powders before SPS(a) SiC particles; (b) Si80Ge20B0.6 matrix; (c) Si80Ge20B0.6 BM, (d) Si80Ge20B0.6 + 0.5vol% SiC BM

Fig. 3 SEM images of fracture surfaces of bulk samples sintered by SPS(a) Si80Ge20B0.6 matrix; (b) Si80Ge20B0.6 BM; (c) Si80Ge20B0.6 + 0.5vol% SiC BM

Fig. 4 TEM images and EDS results of Si80Ge20B0.6 + 0.5vol% SiC BM sample(a) TEM image of the composite containing nano-SiC; (b) EDS of the region at areas I and II in (a); (c) High magnification of the sub-region in (a); (d) HRTEM image of the interface between Si80Ge20B0.6 matrix and nano-SiC particle; (e, f) HRTEM images of Si80Ge20B0.6 matrix and nano-SiC particle, respectively; (g, h) Fourier transfer diffraction patterns of (e) and (f), respectively

Fig. 5 Temperature dependence of (a) electrical conductivity, (b) Seebeck coefficient, (c) power factor and (d) carrier concentration for Si80Ge20B0.6 matrix, Si80Ge20B0.6 BM and Si80Ge20B0.6 + xvol% SiC BM (x = 0.3, 0.5, 1.0) samples

Table 1 Room temperature carrier concentration and mobility for Si80Ge20B0.6 matrix, Si80Ge20B0.6 BM and Si80Ge20B0.6 + xvol% SiC BM (x = 0.3, 0.5, 1.0) samples

Sample	Carrier concentration/ (×10²⁰, cm^-3)	Carrier mobility/ (cm²·V^-1·s^-1)
Si₈₀Ge₂₀B_0.6 matrix	3.4	36
Si₈₀Ge₂₀B_0.6 BM	1.4	30
Si₈₀Ge₂₀B_0.6 + 0.3vol% SiC BM	1.3	28
Si₈₀Ge₂₀B_0.6 + 0.5vol% SiC BM	1.3	26
Si₈₀Ge₂₀B_0.6 + 1.0vol% SiC BM	1.4	23

Fig. 6 Temperature dependence of (a) thermal conductivity and (b) lattice thermal conductivity for Si80Ge20B0.6 matrix, Si80Ge20B0.6 BM and Si80Ge20B0.6 + xvol% SiC BM (x = 0.3, 0.5, 1.0) samples

Fig. 7 Temperature dependence of ZT values for RTG p-type Si80Ge20 alloy[3], Si80Ge20B0.6 matrix, Si80Ge20B0.6 BM and Si80Ge20B0.6 + xvol% SiC BM (x = 0.3, 0.5, 1.0) samples

参考文献 23

[1]	SLACK G A, HUSSAIN M A.The maximum possible conversion efficiency of silicon-germanium thermoelectric generators.Journal of Applied Physics, 1991, 70(5): 2694-2718.
[2]	STEELE M C, ROSI F D.Thermal conductivity and thermoelectric power of germanium-silicon alloys.Journal of Applied Physics, 1958, 29(11): 1517-1520.
[3]	VINING C B.A model for the high-temperature transport-properties of heavily doped n-type silicon-germanium alloys.Journal of Applied Physics, 1991, 69(1): 331-341.
[4]	ROWE D M, ed. CRC Handbook of Thermoelectrics. Boca Raton: CRC Press, 1995, chap. 28.
[5]	VINING C B, LASKOW W, HANSON J O, et al.Thermoelectric properties of pressure-sintered Si0.8Ge0.2 thermoelectric alloys.Journal of Applied Physics, 1991, 69(8): 4333-4340.
[6]	KUNDU A, MINGO N, BROIDO D A, et al. Role of light and heavy embedded nanoparticles on the thermal conductivity of SiGe alloys. Physical Review B, 2011, 84(12): 125426-1-5.
[7]	ROWE D M, SHUKLA V S, SAVVIDES N.Phonon scattering at grain boundaries in heavily doped fine-grained silicon-germanium alloys.Nature, 1981, 290: 765-766.
[8]	SHI L H, JIANG J J, ZHANG G, et al. High thermoelectric figure of merit in silicon-germanium superlattice structured nanowires. Applied Physics Letters, 2012, 101(23):233114/1-233114/4.
[9]	LU J B, GUO R Q, DAI W J, et al.Enhanced in-plane thermoelectric figure of merit in p-type SiGe thin films by nanograin boundaries.Nanoscale, 2015, 7: 7331-7339.
[10]	MINNICH A J, DRESSELHAUS M S, REN Z F, et al.Bulk nanostructured thermoelectric materials: current research and future prospects.Energy & Environmental Science, 2009, 2: 466-479.
[11]	DRESSELHAUS M S, CHEN G, TANG M Y, et al.New directions for low dimensional thermoelectric materials.Advanced Materials, 2007, 19(8): 1043-1053.
[12]	JOSHI G, LEE H, LAN Y C, et al.Enhanced thermoelectric figure-of-merit in nanostructured p-type silicon germanium bulk alloys.Nano Letters, 2008, 8(12): 4670-4674.
[13]	WANG X W, LEE H, LN Y C, et al. Enhanced thermoelectric figure of merit in nanostructured n-type silicon germanium bulk alloy. Journal of Applied Physics, 2008, 93(19): 193121-1-3.
[14]	BASU R, BHATTACHARYA S, BHATT R, et al.Improved thermoelectric performance of hot pressed nanostructured n-type SiGe bulk alloys.Journal of Materials Chemistry A, 2014, 2(19): 6922-6930.
[15]	BATHULA S, JAYASIMHADRI M, GAHTORI B, et al.The role of nanoscale defect features in enhancing the thermoelectric performance of p-type nanostructured SiGe alloys.Nanoscale, 2015, 7(29): 12474-12483.
[16]	BATHULA S, JAYASIMHADRI M, SINGH N, et al. Enhanced thermoelectric figure-of-merit in spark plasma sintered nanostructured n-type SiGe alloys. Applied Physics Letters, 2012,101(21):213902/1-213902/5.
[17]	POUDEL B, HAO Q, MA Y, LAN Y, et al.High-thermoelectric performance of nanostructured bismuth antimony telluride bulk alloys.Science, 2008, 320(5876): 634-638.
[18]	ZHOU X, WANG G, ZHANG L, et al.Enhanced thermoelectric properties of Ba-filled skutterudites by grain size reduction and Ag nanoparticle inclusion.Journal of Materials Chemistry, 2012, 22: 2958-2964.
[19]	ZHAO X Y, SHI X, CHEN L D, et al. Synthesis of YbyCo4Sb12/Yb2O3 composites and their thermoelectric properties. Applied Physics Letters, 2006, 89(9): 092121-1-3.
[20]	DING J, LIU R H, GU H, et al.Study on the high temperature stability of YbyCo4Sb12/Yb2O3 composite thermoelectric material. Journal of Inorganic Materials, 2014, 29(2): 209-214.
[21]	LI J, TAN Q, LI J, et al.BiSbTe-based nanocomposites with high ZT: the effect of SiC nanodispersion on thermoelectric properties.Advanced Functional Materials, 2013, 23(35): 4317-4323.
[22]	MINGO N, HAUSER D, KOBAYASHI NP, et al."Nanoparticle-in-Alloy" approach to efficient thermoelectrics: silicides in SiGe.Nano Letters, 2009, 9(2): 711-715.
[23]	FAVIER K, BERNARD-GRANGER G, NAVONE C, et al.Influence of in situ formed MoSi2 inclusions on the thermoelectrical properties of an N-type silicon-germanium alloy.Acta Material, 2014, 64: 429-442.

P型Si₈₀Ge₂₀B_0.6-SiC纳米复合材料的微观结构与热电性能研究

Microstructure and Thermoelectric Properties of p-type Si₈₀Ge₂₀B_0.6-SiC Nanocomposite

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