Sb掺杂对N型half-Heusler材料热电性能的影响

doi:10.15541/jim20130659

无机材料学报 ›› 2014, Vol. 29 ›› Issue (9): 931-935.DOI: 10.15541/jim20130659 CSTR: 32189.14.10.15541/jim20130659

Sb掺杂对N型half-Heusler材料热电性能的影响

樊毅^{1, 2}, 李小亚², 蒋永锋¹, 包晔峰¹

(1. 河海大学常州校区机电工程学院, 常州213022; 2. 中国科学院上海硅酸盐研究所中国科学院能量转换重点实验室, 上海200050)

收稿日期:2013-12-12 修回日期:2014-02-07 出版日期:2014-09-17 网络出版日期:2014-08-21
作者简介:樊毅(1988–), 男, 硕士研究生. E-mail: wdfan_123@126.com
基金资助:
国家自然科学基金(51372261);国家基础研究项目(2013CB632504)

Effect of Sb Doping on Thermoelectric Property of N-type Half-Heusler Compounds

FAN Yi^1,2, LI Xiao-Ya², JIANG Yong-Fen¹, BAO Ye-Feng¹

(1. Mechanical and Electrical Engineering Institute, Changzhou Campus Hohai University, Changzhou 213022, China; 2. CAS Key Laboratory for Energy Conversion Materials, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China)

Received:2013-12-12 Revised:2014-02-07 Published:2014-09-17 Online:2014-08-21
About author:FAN Yi. E-mail: wdfan_123@126.com
Supported by:
National Natural Science Foundation of China (51372261);National Basic Research program of China (2013CB632504)

摘要/Abstract

摘要：

研究了Sb掺杂对N型half-Heusler化合物Zr_0.25Hf_0.25Ti_0.5NiSn_1-_xSb_x (x=0、0.002、0.005、0.01、0.02、0.03)热电传输特性的影响。结果显示, 随着Sb掺杂量增加, 材料的载流子浓度提高, 电阻率降低, 尤其是低温(<300 K)电阻率下降显著, 赛贝克系数降低, 且取得最大赛贝克系数的温度向高温端移动, 最大功率因子增加~20%, 材料的热导率增大, 主要是电子热导率提高的贡献, 晶格热导率影响不大; 当Sb掺杂量较低时(x<0.01), 材料的最大热电性能优值ZT值在0.77左右, 掺杂量x=0.005的样品ZT值在整个温度区间内最优。

关键词: N型Half-Heusler, Sb掺杂, 热电传输特性

Abstract:

The effect of Sb doping on thermoelectric transport properties of N-type half-Heusler compounds Zr_0.25Hf_0.25Ti_0.5NiSn_1-_xSb_x (x=0, 0.002, 0.005, 0.01, 0.02, 0.03) was studied. Results show that with increasing Sb doping amount, the carrier concentration of the samples increases while the electrical resistivity decreases, especially sharply at low temperature range (~300 K). The Seebeck coefficient decreases, and the temperatures at which the Seebeck coefficient reaches climax move to higher ones. Therefore, the power factor increases by ~20%. The total thermal conductivity increases mainly due to the enhancement of electrical thermal conductivity, the lattice thermal conductivity remains almost unchanged. For the samples with x<0.01, the maximum ZT value is about 0.77 at 800 K, and among the samples, the one with x=0.005 performs the best in the whole temperature range.

Key words: N-type half-Heusler, Sb doping, thermoelectric transport property

中图分类号:

O482
TN37

樊毅, 李小亚, 蒋永锋, 包晔峰. Sb掺杂对N型half-Heusler材料热电性能的影响[J]. 无机材料学报, 2014, 29(9): 931-935.

FAN Yi, LI Xiao-Ya, JIANG Yong-Fen, BAO Ye-Feng. Effect of Sb Doping on Thermoelectric Property of N-type Half-Heusler Compounds[J]. Journal of Inorganic Materials, 2014, 29(9): 931-935.

图/表 8

表1 N型Half-Heusler体系的最佳Sb掺杂量

Table 1 The optimal Sb doping amount in different N-type Half-Heusler systems

Systems	Optimal Sb doping amount	Reference
Zr_0.5Hf_0.5NiSn_1-_xSb_x	0.005-0.010	[1]
TiNiSn_1-_xSb_x	0.01-0.05	[6]
Zr_0.25Hf_0.25Ti_0.5NiSn_1-_xSb_x	0.002	[7]
Zr_0.25Hf_0.25Ti_0.5NiSn_1-_xSb_x	0.002	[8]
Hf_0.75Zr_0.25NiSn_1-_xSb_x	0.025	[9]
Hf_0.6Zr_0.4NiSn_1-_xSb_x	0.020	[10]
Hf_0.75Zr_0.25NiSn_1-_xSb_x	0.010	[11]

图1 Zr0.25Hf0.25Ti0.5NiSn1-xSbx(x=0~0.03) SPS烧结样品的XRD图谱

Fig. 1 XRD patterns of the SPSed samples of Zr0.25Hf0.25Ti0.5 NiSn1-x Sbx (x=0-0.03)

图2 Zr0.25Hf0.25Ti0.5NiSn1-xSbx(x=0~0.03)样品载流子浓度随温度的变化

Fig. 2 Temperature dependence of carrier concentration for the Zr0.25Hf0.25Ti0.5NiSn1-xSbx(x=0-0.03) samples

图3 Zr0.25Hf0.25Ti0.5NiSn1-xSbx(x=0~0.03)样品电阻率随温度的变化

Fig. 3 Temperature dependence of electrical resistivity for the Zr0.25Hf0.25Ti0.5NiSn1-xSbx(x=0-0.03) samples

图4 Zr0.25Hf0.25Ti0.5NiSn1-xSbx(x=0~0.03)样品塞贝克系数随温度的变化

Fig. 4 Temperature dependence of Seebeck coefficients for the Zr0.25Hf0.25Ti0.5NiSn1-xSbx(x=0-0.03) samples

图5 Zr0.25Hf0.25Ti0.5NiSn1-xSbx(x=0~0.03)样品功率因子随温度的变化

Fig. 5 Temperature dependence of power factor for the Zr0.25Hf0.25Ti0.5NiSn1-xSbx(x=0-0.03) samples

图6 Zr0.25Hf0.25Ti0.5NiSn1-xSbx(x=0~0.03)样品热导率随温度的变化

Fig. 6 Temperature dependence of thermal conductivity for the Zr0.25Hf0.25Ti0.5NiSn1-xSbx(x=0~0.03) samples (a) Total thermal conductivity; (b) Lattice and electronic contribution to the total thermal conductivity

图7 Zr0.25Hf0.25Ti0.5NiSn1-xSbx(x=0~0.03)样品的热电性能优值ZT值随温度的变化

Fig. 7 Temperature dependence of figure of merit, ZT value for the Zr0.25Hf0.25Ti0.5NiSn1-xSbx(x=0~0.03) samples

参考文献 15

[1]	UHER C, YANG J, HU S, et al. Transport properties of pure and doped MNiSn (M=Zr,Hf). Phys. Rev. B, 1999, 59(13): 8615-8621.
[2]	SHEN Q, CHEN L, GOTO T, et al. Effects of partial substitution of Ni by Pd on the thermoelectric properties of ZrNiSn-based half- Heusler compounds. Appl. Phys. Lett., 2001, 79: 4165.
[3]	MASTRONARDI K, YONG D, WANG C C, et al. Antimonides with the half-Heusler structure: new thermoelectric materials. Appl. Phys. Lett., 1999, 74: 1415.
[4]	ALIEV F G, KOZYRKOV V V, MOSHCHALKOV V V, et al. Narrow band in the intermetallic compounds MNiSn (M = Ti, Zr, Hf). Z. Phys. B, 1990, 80(3): 353-357.
[5]	HOHL H, RAMIREZ A P, GOLDMANN C, et al. Efficient dopants for ZrNiSn-based thermoelectric materials. J. Phys. Condens. Matter., 1999, 11(7): 1697-1709.
[6]	BHATTACHARYA S, TRITT M T, XIA Y, et al. Grain structure effects on the lattice thermal conductivity of Ti-based half-Heusler alloys. Appl. Phys. Lett., 2002, 81: 43-45.
[7]	SAKURADA S, SHUTOH N. Effect of Ti substitution on the thermoelectric properties of (Zr,Hf)NiSn half-Heusler compounds. Appl. Phys. Lett. , 2005, 86(8): 082105-1-3.
[8]	MICHAEL S, BENJAMIN B. Phase separation as a key to a thermoelectric high efficiency. Phys. Chem. Chem. Phys., 2013, 15: 1868.
[9]	SLADE R, POON SJ, HICKMAN N, et al. Effect of substitutions on the thermoelectric figure of merit of half-Heusler phases at 800℃. Appl. Phys. Lett. , 2006, 88(4): 042106-1-3.
[10]	YU C, ZHU T J, SHI R Z, et al. High-performance half-Heusler thermoelectric materials Hf1-xZrxNiSn1-ySby prepared by levitation melting and spark plasma sintering. Acta Materialia, 2009, 57: 2757-2764.
[11]	JOSHI GIRI, YAN XIAO, WANG HENGZHI, et al. Enhancement in thermoelectric figure-of-merit of an N-type half-Heusler compound by the nanocomposite approach. Advanced Energy Materials. 2011, 1: 643-647.
[12]	NOLAS G S, SHARP J, GOLDSMID H J. Thermoelectrics: Basic Principles and New Materials Developments, Berlin: Springer- Verlag, 2001: 51-55.
[13]	BIRKEL C S, DOUGLAS J E, LETTIERE B R, et al. Improving the thermoelectric properties of half-Heusler TiNiSn through inclusion of a second full-Heusler phase: microwave preparation and spark plasma sintering of TiNi1+xSn. Phys. Chem. Chem. Phys., 2013, 15: 6990-6997.
[14]	黄昆,韩汝琦. 半导体物理基础. 北京: 科学出版社, 1979: 64-67.
[15]	高敏,张景韶,ROWE D M. 温差电转换及其应用. 北京: 兵器工业出版社, 1996: 51-52.

Sb掺杂对N型half-Heusler材料热电性能的影响

Effect of Sb Doping on Thermoelectric Property of N-type Half-Heusler Compounds

RichHTML

PDF (PC)

可视化

摘要/Abstract

引用本文

使用本文

图/表 8

参考文献 15

相关文章 4

编辑推荐

Metrics

本文评价

[1]	孔国强, 冷明哲, 周战荣, 夏池, 沈晓芳. Sb掺杂O3型Na_0.9Ni_0.5Mn_0.3Ti_0.2O₂钠离子电池正极材料[J]. 无机材料学报, 2023, 38(6): 656-662.
[2]	韩志明, 张忻, 路清梅, 张久兴, 张飞鹏. (Mg₂Si_1-xSb_x)_0.4-(Mg₂Sn)_0.6固溶体合金的制备及热电输运特性[J]. 无机材料学报, 2012, 27(8): 822-826.
[3]	祝柏林,曾大文,谢长生,胡木林,宋武林. 蒸气氧化法制备掺锑氧化锌纳米颗粒的研究[J]. 无机材料学报, 2003, 18(6): 1255-1260.
[4]	郭玉忠,王剑华,黄瑞安,王贵青. 掺杂SnO₂透明导电薄膜电学及光学性能研究[J]. 无机材料学报, 2002, 17(1): 131-138.