无机材料学报 ›› 2024, Vol. 39 ›› Issue (8): 895-902.DOI: 10.15541/jim20240012
程俊1,2(), 张家伟1,2(), 仇鹏飞1,2,3, 陈立东1,2, 史迅1,2()
收稿日期:
2024-01-08
修回日期:
2024-03-04
出版日期:
2024-08-20
网络出版日期:
2024-03-22
通讯作者:
张家伟, 研究员. E-mail: jiaweizhang@mail.sic.ac.cn;作者简介:
程 俊(1997-), 男, 博士研究生. E-mail: chengjun@student.sic.ac.cn
基金资助:
CHENG Jun1,2(), ZHANG Jiawei1,2(), QIU Pengfei1,2,3, CHEN Lidong1,2, SHI Xun1,2()
Received:
2024-01-08
Revised:
2024-03-04
Published:
2024-08-20
Online:
2024-03-22
Contact:
ZHANG Jiawei, professor. E-mail: jiaweizhang@mail.sic.ac.cn;About author:
CHENG Jun (1997-), male, PhD candidate. E-mail: chengjun@student.sic.ac.cn
Supported by:
摘要:
β-FeSi2作为一种绿色环保、高温抗氧化的热电材料, 在工业余热回收领域具有潜在的应用价值。虽然磷(P)是一种理想的β-FeSi2硅(Si)位的n型掺杂元素, 但是P掺杂β-FeSi2易出现第二相, 从而限制了其热电性能的提升。本研究采用感应熔炼法合成了一系列FeSi2-xPx (x=0, 0.02, 0.04, 0.06)样品, 极大程度地避免了第二相的产生, 并系统研究了P掺杂对β-FeSi2热电输运性能的影响。结果表明, P在β-FeSi2中的掺杂极限约为0.04, 与前期的理论缺陷计算结果相符。此外, P掺杂优化了β-FeSi2的热电性能, 在850 K时, FeSi1.96P0.04的最高热电优值ZT约为0.12, 远高于已有的研究结果(673 K, 最高ZT仅为0.03)。然而, 与同为n型Co和Ir掺杂的β-FeSi2相比(其载流子浓度可达1022 cm-3), P掺杂β-FeSi2的载流子浓度较低, 最高仅为1020 cm-3, 这导致其电声散射效应较弱, 从而限制了整体热电性能的提升。若能提高其载流子浓度, 则热电性能有望得到进一步提升。
中图分类号:
程俊, 张家伟, 仇鹏飞, 陈立东, 史迅. P掺杂β-FeSi2材料的制备与热电输运性能[J]. 无机材料学报, 2024, 39(8): 895-902.
CHENG Jun, ZHANG Jiawei, QIU Pengfei, CHEN Lidong, SHI Xun. Preparation and Thermoelectric Transport Properties of P-doped β-FeSi2[J]. Journal of Inorganic Materials, 2024, 39(8): 895-902.
图1 (a) FeSi2-xPx (x=0, 0.02, 0.04, 0.06)的室温XRD图谱和(b) β-FeSi2的晶体结构示意图
Fig. 1 (a) Room-temperature XRD patterns of FeSi2-xPx (x=0, 0.02, 0.04, 0.06) and (b) crystal structure of β-FeSi2
图2 FeSi2-xPx (x=0.02, 0.04, 0.06)的SEM照片和对应的EDS元素分布图
Fig. 2 SEM images of as-synthesized FeSi2-xPx (x=0.02, 0.04, 0.06) and corresponding EDS elemental mappings
图3 样品的电输运性能
Fig. 3 Electrical transport properties of samples (a, b) Temperature dependences of electrical conductivity σ (a) and Seebeck coefficient S (b) for as-synthesized FeSi2-xPx (x=0, 0.02, 0.04, 0.06); (c, d) Comparison of the absolute values of Seebeck coefficients |S| (c) and carrier concentrations nH (d) for Co-, Ir-, and P-doped β-FeSi2 at 300 K; (e) Temperature dependence of power factor PF for as-synthesized FeSi2-xPx (x=0, 0.02, 0.04, 0.06); (f) Comparison of room-temperature power factor PF for various n-type doped β-FeSi2[13-14,17 -18,25]; Colorful figures are available on website
图4 样品的热输运性能
Fig. 4 Thermal transport properties of samples (a, b) Temperature dependences of total thermal conductivity κ (a) and lattice thermal conductivity κL (b) for as-synthesized FeSi2-xPx (x=0, 0.02, 0.04, 0.06); (c) Temperature dependence of the experimental and Debye model calculated lattice thermal conductivity κL for as-synthesized FeSi1.96P0.04 (U: Umklapp process; B: grain-boundary scattering; PD: point-defect scattering; EP: phonon-electron scattering); (d) Comparison of room temperature lattice thermal conductivity κL for Co-, Ir-, and P-doped β-FeSi2 at the same doping content; (e, f) Room-temperature lattice thermal conductivity κL as a function of the doping content of Co-doped β-FeSi2 (e) and P-doped β-FeSi2 (f), in which the solid square symbols represent the experimental data, while the red solid lines denote the Callaway model; Colorful figures are available on website
图5 样品的总热电性能
Fig. 5 Overall thermoelectric performance of samples (a) Temperature dependence of ZT for as-synthesized FeSi2-xPx (x=0, 0.02, 0.04, 0.06); (b) Comparison on ZT values of various n-type doped β-FeSi2[13-14,17 -18,25]
Fitting parameter | FeSi1.96P0.04 |
---|---|
L/μm | 3 |
A/(×10-41, s3) | 0.09 |
B/(×10-18, s·K-1) | 0.48 |
C/(×10-15, s-1) | 0.08 |
R2 | 0.99642 |
χ2 | 0.06560 |
表S1 FeSi1.96P0.04的晶格热导率拟合参数
Table S1 Parameters used to fit the lattice thermal conductivity κL of FeSi1.96P0.04
Fitting parameter | FeSi1.96P0.04 |
---|---|
L/μm | 3 |
A/(×10-41, s3) | 0.09 |
B/(×10-18, s·K-1) | 0.48 |
C/(×10-15, s-1) | 0.08 |
R2 | 0.99642 |
χ2 | 0.06560 |
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