(Ag2Se)1-x(Bi2Se3)x的热电性能研究

doi:10.15541/jim20180249

摘要/Abstract

摘要：

具有本征低晶格热导率的I-V-VI₂族三元硫属化合物在热电领域引起了广泛关注。AgBiSe₂作为这类化合物中少有的n型半导体, 成为一种有潜力的热电材料。本工作系统研究了AgBiSe₂的热电性能。基于Ag₂Se-Bi₂Se二元相图, 单相的(Ag₂Se)_1-_x(Bi₂Se₃)_x的成分在x=0.4~0.62范围可调, 使得该材料载流子浓度具有可调性。结果表明, 通过组分调控获得了较宽范围的载体浓度1.0×10¹⁹~5.7×10¹⁹ cm^-3, 并基于声学声子散射的单一抛物带模型对其电传输性能进行了综合评估。本研究获得的最高载流子浓度接近理论最优值, 在700 K实现了最高ZT值0.5。本研究有助于深入理解AgBiSe₂的传输特性和决定热电性能的基本物理参数。

关键词: 热电材料, 热电性能, AgBiSe₂, 载流子浓度, SPB模型

Abstract:

Ternary chalcogenides I-V-VI₂ compounds attract extensive attentions for thermoelectric applications due to their intrinsically low lattice thermal conductivity. AgBiSe₂, as one of a few n-type semiconductors among these compounds, shows the potential to be a promising thermoelectric material. Therefore, this work focuses on its thermoelectric properties. According to the phase diagram of Ag₂Se-Bi₂Se₃ system, the single phase region of (Ag₂Se)_1-_x(Bi₂Se₃)_x allows x to be varied in the range of 0.4~0.62. This large variation of x suggests a tunability of carrier concentration for this material. A broad carrier concentration of 1.0×10¹⁹~5.7×10¹⁹ cm^-3 for single phased (Ag₂Se)_1-_x(Bi₂Se₃)_x is obtained through a composition manipulation, which enables a comprehensive assessment on electronic transport properties based on a single parabolic band model with acoustic scattering. The highest carrier concentration obtained in this work, approaching to the theoretical optimal one, leads to a peak ZT of 0.5 at 700 K. This work offers a well understanding of its transport properties and underlying physical parameters determining the thermoelectric performance.

Key words: thermoelectric material, thermoelectric properties, AgBiSe₂, carrier concentration, SPB model

中图分类号:

TB34

刘虹霞, 李文, 张馨月, 李娟, 裴艳中. (Ag₂Se)_1-_x(Bi₂Se₃)_x的热电性能研究[J]. 无机材料学报, 2019, 34(3): 341-348.

LIU Hong-Xia, LI Wen, ZHANG Xin-Yue, LI Juan, PEI Yan-Zhong. Thermoelectric Properties of (Ag₂Se)_1-_x(Bi₂Se₃)_x[J]. Journal of Inorganic Materials, 2019, 34(3): 341-348.

图/表 9

Fig. 1 Crystal structures for the different phases of AgBiSe2 (a) and phase diagram of Ag2Se-Bi2Se3 system (b)[57]

Fig. 2 Powder XRD patterns for (Ag2Se)1-x(Bi2Se3)x(0.4≤x≤0.62)

Fig. 3 Locally enlarged XRD patterns (a) and composition dependent lattice parameters (b) for the samples with 0.48≤x≤0.56

Fig. 4 SEM images for (Ag2Se)1-x(Bi2Se3)x(0.48≤x≤0.56) (a, c-g) and its corresponding EDS mapping for the samples with x=0.48 (b) and 0.58 (h)

Fig. 5 Composition dependent Hall carrier concentration (a) and normalized optical absorption versus photon energy (b) at room temperature for (Ag2Se)1-x(Bi2Se3)x(0.5≤x≤0.56)

Fig. 6 Temperature dependent Hall coefficient (RH) and mobility (µH) (a), deformation potential coefficient (Edef) and density of states effective mass (m*) (b), Hall carrier concentration dependent Hall mobility (c) and Seebeck coefficient (d) at different temperatures for (Ag2Se)1-x(Bi2Se3)x(0.5≤x≤0.56), with a comparison to available literature results[52,64-65]. The experimental results here agree well with the model prediction based on a SPB approximation with a dominant scattering by acoustic phonons

Fig. 7 Temperature dependent Seebeck coefficient (a), electrical resistivity (b), total thermal conductivity (c) and lattice thermal conductivity (d) for (Ag2Se)1-x(Bi2Se3)x(0.5≤x≤0.56), with a comparison to available literature results[63,64]

Table 1 Measured sound velocities and the estimated physical parameters for (Ag2Se)1-x(Bi2Se3)x(0.5≤x≤0.56)

(Ag₂Se)_1-_x(Bi₂Se₃)_x	ν_T/(m•s^-1)	ν_L/(m•s^-1)	ν_s/(m•s^-1)	B/ GPa	γ	θ_D/K
x=0.5	1390	2560	1550	31.5	1.7	158
x=0.51	1410	2610	1570	32.4	1.7	159
x=0.52	1360	2500	1520	29.6	1.7	154
x=0.54	1290	2660	1450	37.8	2.1	146
x=0.56	1380	2760	1550	39.8	2.0	156

Fig. 8 Temperature dependent ZT for (Ag2Se)1-x(Bi2Se3)x(0.5≤x≤0.56) (a) and Hall carrier concentration dependentZT at different temperatures (b) with a comparison to model prediction and literature results[52,63-65]

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(Ag₂Se)_1-_x(Bi₂Se₃)_x的热电性能研究

Thermoelectric Properties of (Ag₂Se)_1-_x(Bi₂Se₃)_x

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