Realizing enhanced thermoelectric properties in Cu2S-alloyed SnSe based composites produced via solution synthesis and sintering

doi:10.1016/j.jmst.2020.10.062

Abstract

Abstract:

SnSe emerges as one of the most promising Te-free thermoelectric materials due to its strong anharmonicity and multiple valence bands structure. Recently, compositing has been proven effective in optimizing thermoelectric performance of various metal chalcogenides. Herein, a series of SnSe-xCu2S (x = 0, 0.5%, 1%, 3%, 5%) materials have been fabricated via solution synthesis, particle blending, and spark plasma sintering in sequence. After incorporating Cu2S, the materials become SnSe based composites with Cu doping, S substitution and Cu2SnSe3 secondary phase. We elucidate that the power factor of polycrystalline SnSe can be tuned and enhanced at varied temperature ranges through adjusting the addition amount of Cu2S. Additionally, the composites achieve suppressed lattice thermal conductivity when compared to SnSe itself, as the introduced point defects and SnSe/Cu2SnSe3 interfaces intensify phonon scattering. Consequently, SnSe-0.5%Cu2S and SnSe-3%Cu2S achieve a peak zT of 0.70 at 830 K (intermediate temperature range) and a highly increased zT of 0.28 at 473 K (low temperature range), respectively, which are ∼130% and 200% of values reached by SnSe at the corresponding temperatures. The study demonstrates that our approach, which combines compositing with elemental doping and substitution, is effective in optimizing the thermoelectric performance of SnSe at varied temperature ranges.

Key words: Thermoelectric, Tin chalcogenides, Solution synthesis, Composites, Transmission electron microscopy

Yao Chen, Jie Chen, Bin Zhang, Meiling Yang, Xiaofang Liu, Hengyang Wang, Lei Yang, Guoyu Wang, Guang Han, Xiaoyuan Zhou. Realizing enhanced thermoelectric properties in Cu₂S-alloyed SnSe based composites produced via solution synthesis and sintering[J]. J. Mater. Sci. Technol., 2021, 78: 121-130.

Figures/Tables 7

Fig. 1. Schematic illustration of the experimental procedures for the fabrication of SnSe-xCu2S (x = 0, 0.5%, 1%, 3%, 5%) pellets.

Fig. 2. XRD patterns for the SnSe-xCu2S (x = 0, 0.5%, 1%, 3%, 5%) sintered pellets measured (a) parallel and (b) perpendicular to the pressing direction (indicated in the insets).

Fig. 3. Cross-sectional SEM images of fractured surfaces for sintered SnSe-xCu2S pellets: (a and d) x = 0.5%, (b and e) x = 3%, (c and f) x = 5%. (a-c) perpendicular and (d-f) parallel to the pressing directions that are indicated by blue arrows in the images. The insets indicate the corresponding pellet orientation and the viewing directions.

Fig. 4. TEM characterization of the SnSe-3%Cu2S sintered sample: (a) HAADF-STEM image, (b) EDS mappings, (c and e) SAED patterns collected from particle “A” and “B” labelled in (a), which are indexed along the [001] zone axis of SnSe and the [011] zone axis of Cu2SnSe3, respectively, (d and f) the corresponding HRTEM images.

Fig. 5. TEM characterization of the SnSe-0.5%Cu2S sintered sample: (a) HAADF-STEM image, (b) EDS elemental maps of Sn, Se, Cu and S, (c) TEM image, HAADF image, EDS mapping of another region, (d) SAED pattern collected from particle “A” in (c), (e) the corresponding HRTEM image.

Fig. 6. Temperature dependent thermoelectric performance of SnSe-xCu2S (x = 0, 0.5%, 1%, 3%, 5%) pellets: (a) electrical conductivity (σ), (b) Seebeck coefficient (S), (c) power factor (S2σ), (d) total (κtot) and (e) lattice (κlat) thermal conductivity, (f) zT.

Table 1 Electrical conductivity (σ), Hall carrier concentration (nH) and carrier mobility (μH) at room temperature of SnSe-xCu2S (x = 0, 0.5%, 1%, 3%, 5%).

SnSe-xCu₂S pellets	σ (S m^-1)	n_H (10¹⁸ cm^-3)	μ_H (cm² V^-1 s^-1)
x = 0	1760	10.9	10.1
x = 0.5%	1260	7.8	10.1
x = 1%	820	5.4	9.5
x = 3%	2850	18.1	9.8
x = 5%	5100	35.1	9.1

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Realizing enhanced thermoelectric properties in Cu₂S-alloyed SnSe based composites produced via solution synthesis and sintering

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