High thermoelectric and mechanical performance in the n-type polycrystalline SnSe incorporated with multi-walled carbon nanotubes

doi:10.1016/j.jmst.2021.12.002

J. Mater. Sci. Technol. ›› 2022, Vol. 114: 55-61.DOI: 10.1016/j.jmst.2021.12.002

• Research Article • Previous Articles Next Articles

High thermoelectric and mechanical performance in the n-type polycrystalline SnSe incorporated with multi-walled carbon nanotubes

Xin-Yu Mao^a, Xiao-Lei Shi^b^,^c, Liang-Chuang Zhai^a, Wei-Di Liu^d, Yue-Xing Chen^e, HanGao ^f, Meng Li^g, De-Zhuang Wang^a, Hao Wu^a, Zhuang-Hao Zheng^e, Yi-Feng Wang^h^,ⁱ, Qingfeng Liu^a^,^j^,^*(), Zhi-Gang Chen^b^,^c^,^*()

^aState Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing 211816, China
^bCentre for Future Materials, University of Southern Queensland, Springfield Central, Brisbane, 4300, Australia
^cSchool of Chemistry and Physics, Queensland University of Technology, Brisbane, QLD 4000, Australia
^dAustralian Institute for Bioengineering and Nanotechnology, The University of Queensland, Brisbane, QLD 4072, Australia
^eShenzhen Key Laboratory of Advanced Thin Films and Applications, Key Laboratory of Optoelectronic Devices and Systems of Ministry of Education and Guangdong Province, College of Physics and Optoelectronic Engineering, Shenzhen University, Shenzhen 518060, China
^fKey Laboratory of Material Physics of Ministry of Education, School of Physics and Microelectronics, Zhengzhou University, Zhengzhou 450052, China
^gSchool of Mechanical and Mining Engineering, The University of Queensland, St Lucia, Brisbane, QLD 4072, Australia
^hCollege of Materials Science and Engineering, Nanjing Tech University, Nanjing 211816, China
ⁱJiangsu Collaborative Innovation Center for Advanced Inorganic Function Composites, Nanjing Tech University, Nanjing 211816, China
^jCAS Key Laboratory of Carbon Materials, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China

Received:2021-10-27 Revised:2021-11-29 Accepted:2021-12-08 Published:2022-07-01 Online:2022-01-13
Contact: Qingfeng Liu,Zhi-Gang Chen
About author:zhigang.chen@qut.edu.au, zhigang.chen@uq.edu.au (Z.-G. Chen).
*E-mail addresses: qfliu@njtech.edu.cn (Q. Liu),
First author contact:
¹These authors contribute equally to this work.

Abstract

Abstract:

In this study, we introduce multi-walled carbon nanotubes (MWCNTs) in Pb/I co-doped n-type polycrystal SnSe to simultaneously improve its thermoelectric and mechanical properties for the first time. The introduced MWCNTs act as the “bridges” to accelerate the electron carrier transport between SnSe grains, leading to significantly increased electrical conductivity from 32.6 to 45.7 S cm^-1 at 773 K, which contributes to an enhanced power factor of ∼5.0 μW cm^-1 K ^{- 2} at this temperature. Although MWCNTs possess high intrinsic thermal conductivities, these MWCNTs, acting as nanoinclusions in the SnSe matrix to form the dense interfaces between SnSe and MWCNTs, provide extra heat-carrying phonon scattering centers, leading to a slightly reduced lattice thermal conductivity of only 0.34 W m ^{- 1} K ^{- 2} at 773 K and in turn, a high ZT of ∼1.0 at this temperature. Furthermore, the introduced MWCNTs can simultaneously act as the “binders” to bond adjacent grains, significantly improving the mechanical properties of SnSe by boosting its Vickers hardness from 39.5 to 50.5. This work indicates that our facile approach can achieve high thermoelectric and mechanical properties in n-type SnSe polycrystals with a considerable potential for applying to thermoelectric devices as n-type elements.

Key words: Thermoelectric property, SnSe, N-type, Multi-walled carbon nanotubes, Mechanical property

Xin-Yu Mao, Xiao-Lei Shi, Liang-Chuang Zhai, Wei-Di Liu, Yue-Xing Chen, HanGao , Meng Li, De-Zhuang Wang, Hao Wu, Zhuang-Hao Zheng, Yi-Feng Wang, Qingfeng Liu, Zhi-Gang Chen. High thermoelectric and mechanical performance in the n-type polycrystalline SnSe incorporated with multi-walled carbon nanotubes[J]. J. Mater. Sci. Technol., 2022, 114: 55-61.

Figures/Tables 5

Fig. 1. (a) Schematic diagram of fabricating PbI2-doped polycrystalline SnSe incorporated with MWCNTs. (b) Illustration of the crystal structure of PbI2-doped SnSe incorporated with MWCNTs. (c) Comparison of temperature-dependent ZT of SnSe0.95, Sn0.97Pb0.03Se0.89I0.06, and Sn0.97Pb0.03Se0.89I0.06 + 1 wt% MWCNTs. (d) Vickers hardness of PbI2-doped SnSe with and without MWCNTs.

Fig. 2. (a) XRD and (b) Raman spectrums of 3% PbI2-doped polycrystalline n-SnSe incorporated with different contents of MWCNTs. (c) Scanning electronic microscopy (SEM) image of cracked n-SnSe incorporated with 1 wt% MWCNTs. (d) SEM image of a typical n-SnSe grain with a layered structure. SEM images of micropores found in n-SnSe grains viewed from the in-plane (e) and out-of-plane (f) directions. (g) SEM image of cracked n-SnSe with MWCNTs. (h) Magnified SEM image of MWCNTs on the surface of one n-SnSe grain. (i) Magnified SEM image of MWCNTs linked between two n-SnSe grains.

Fig. 3. (a) Spherical aberration-corrected scanning transmission electron microscopy (Cs-STEM) high-angle annular dark-field (HAADF) image of n-SnSe to show grain boundaries. (b) Corresponding energy dispersive spectroscopy (EDS) maps of Sn, Se, Pb, and I. (c) STEM image of the n-SnSe matrix to show some nanoprecipitates with different contrast from the matrix. (d) TEM image of the contrast interface between n-SnSe matrix and nanoprecipitate. (e) Corresponding selected area electron diffraction (SAED) pattern of (d). (f) High-resolution TEM (HRTEM) image of n-SnSe matrix. (g) HRTEM image of the interfaces between n-SnSe matrix and MWCNT. (h) Corresponding SAED pattern of (g). (i) Calculated spectral lattice thermal conductivity (κs) of n-SnSe with 1 wt% MWCNTs at 300 K using the Debye-Callaway model.

Fig. 4. T-dependent (a) electrical conductivity σ, (b) Seebeck coefficient S, and (c) power factor S2σ of the n-SnSe incorporated with MWCNTs. (d) Electron carrier concentration ne and mobility μ, (e) effective mass m*, and (f) ne-dependent S2σ of n-SnSe incorporated with MWCNTs. All properties are measured or determined along the direction perpendicular to the sintering pressure.

Fig. 5. T-dependent (a) thermal conductivity κ, (b) electronic thermal conductivity κe, and (c) lattice thermal conductivity κl of n-SnSe incorporated with different contents of MWCNTs. (d) 1000/T-dependent κl, (e) T-dependent ZT, and (f) ne-dependent ZT of n-SnSe incorporated with different contents of MWCNTs. All properties are measured or determined along the direction perpendicular to the sintering pressure.

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High thermoelectric and mechanical performance in the n-type polycrystalline SnSe incorporated with multi-walled carbon nanotubes

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