放量制备Ba、Yb填充方钴矿(Ba,Yb)yCo4Sb12的热电性能
Thermoelectric Properties of Scaled-Up Double-Filled (Ba,Yb)yCo4Sb12 Skutterudites

作者: 宋海东 , 包晔峰 :河海大学,江苏 南京; 李小亚 :中国科学院上海硅酸盐研究所,中科院能源转换材料重点实验室,上海;

关键词: (BaYb)填充方钴矿放量制备热电性能(BaYb) Filled Skutterudites Amplification Preparation Thermoelectric Properties

摘要:
热电性能研究通常只需要制备2~3克材料,而热电器件的研制和应用需要大量的材料。为了获得放量制备的高性能热电材料,本文采用熔融、淬火、退火结合放电等离子烧结技术放量制备了Ba、Yb填充方钴矿(Ba,Yb)yCo4Sb12,研究了Ba、Yb填充原子加入量对材料相组成、填充量及其热电性能的影响。结果表明,放量制备的(Ba,Yb)yCo4Sb12填充方钴矿材料主要由方钴矿相和微量的YbSb组成;随着填充原子加入量增加,材料的实际填充量增大,电阻率、赛贝克系数绝对值减小,晶格热导率大幅度降低;放量制备的(Ba,Yb)yCo4Sb12材料的最大ZT值达到1.31 (850 K时),接近报道的最高值。

Abstract: It usually needs about two grams thermoelectric materials to study their performance, while more are needed to develop and apply their devices. To obtain high performance scaled up barium and ytterbium filled skutterudites, we scaled up (Ba,Yb)yCo4Sb12 (y = 0.1, 0.12, 0.15) skutterudites by melting, quenching, annealing and spark plasma sintering, and studied the effects of the added amount of barium and ytterbium on the phase composition, filling fraction of barium and ytter- bium and thermoelectric properties of the materials. Results show that the scaled up (Ba,Yb)yCo4Sb12 materials consist of mainly skutterudite phase and trace amount of YbSb phase. With the added amount of barium and ytterbium increasing, the real filling fraction of barium and ytterbium increases, the resistivity and the absolute Seebeck coefficient of the skutterudits decreases and the lattice thermal conductivity of the materials drops sharply. The maximum ZT for the (Ba,Yb)yCo4Sb12 material reaches 1.31 at 850 K, close to the highest value reported.

文章引用: 宋海东 , 包晔峰 , 李小亚 (2015) 放量制备Ba、Yb填充方钴矿(Ba,Yb)yCo4Sb12的热电性能。 凝聚态物理学进展, 4, 10-17. doi: 10.12677/CMP.2015.41002

参考文献

[1] Nolas, G.S., Morelli, D.T. and Tritt Terry, M. (1999) Skutterudites: A phonon-glass-electron crystal approach to ad-vanced thermoelectric energy conversion applications. Annual Reviews, 29, 89-116.

[2] Shi, X., Zhang, W., Chen, L.D., et al. (2005) Filling fraction limit for intrinsic voids in crystals: doping in skutterudites. Physical Review Letters, 18, Article ID: 185503.

[3] Feldman, J.L., Dai, P.C., Enck, T., et al. (2006) Lattice vibrations in La(Ce)Fe4Sb12 and CoSb3: Inelastic neutron scattering and theory. Physical Review B, 1, Article ID: 014306.

[4] Bai, S.Q., Shi, X. and Chen, L.D. (2010) Lattice thermal transport in BaxREyCo4Sb12 (RE=Ce, Yb, and Eu) double- filled skutterudites. Applied Physics Letters, 20, Article ID: 202102.

[5] Li, H., Tang, X.F., Zhang, Q.J., et al. (2008) Rapid preparation method of bulk nanostructure Yb0.3Co4Sb12+y compounds and improved thermoelectric performance. Applied Physics Letters, 25, Article ID: 252109.

[6] Shi, X., Kong, H., Li, C.P., et al. (2008) Low thermal conductivity and high thermoelectric figure of merit in n-type BaxYbyCo4Sb12 double-filled skutterudites. Applied Physics Letters, 18, Article ID: 182101.

[7] Shi, X., Yang, J., Salvador, J.R., et al. (2011) Multiple-filled skutterudites: high thermoelectric figure of merit through separately optimizing electrical and thermal transports. Journal of the American Chemical Society, 133, 7837-7846.

[8] Nolas, G.S., Kaeser, M., Littleton, I.V.R.T., et al. (2000) High figure of merit in partially filled ytterbium skutterudite materials. Applied Physics Letters, 12, 1855-1857.

[9] Sedat, B. and Strirad, U. (2014) Enhanced thermoelectric performance of optimized Ba, Yb filled and Fe substituted skutterudite compounds. Journal of Alloys and Compounds, 585, 168-172.

[10] Wu, T., Bai, S.Q., Shi, X., et al. (2013) Enhanced thermoelectric properties of BaxEuyCo4Sb12 with very high filling fraction. Journal of Inorganic Materials, 2, 224-228.

[11] Peng, J.Y., He, J., Su, Z., et al. (2009) High temperature thermoelectric properties of double-filled InxYbyCo4Sb12 skutterudites. Journal of Applied Physics, 8, Article ID: 084907.

[12] Zhao, W.Y., Dong, C.L., Wei, P., et al. (2007) Synthesis and high temperature transport properties of barium and in- dium double-filled skutterudites BaxInyCo4Sb12-z. Journal of Applied Physics, 11, Article ID: 113708.

[13] Bai, S.Q., Pei, Y.Z., Chen, L.D., et al. (2009) Enhanced thermoelectric performance of dual-element-filled skutteru- dites BaxCeyCo4Sb12. Acta Materialia, 57, 3135-3139.

分享
Top