Journal
KOREAN JOURNAL OF METALS AND MATERIALS
Volume 59, Issue 10, Pages 736-743Publisher
KOREAN INST METALS MATERIALS
DOI: 10.3365/KJMM.2021.59.10.736
Keywords
thermoelectric; tetrahedrite; mechanical alloying; hot pressing
Funding
- Basic Science Research Capacity Enhancement Project (National Research Facilities and Equipment Center) through the Korea Basic Science Institute - Ministry of Education [2019R1A6C1010047]
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In this study, tetrahedrite compounds doped with Sn were successfully prepared and analyzed for their charge transport and thermoelectric properties. The results showed that increasing Sn content led to higher Seebeck coefficient and power factor, but lower electrical conductivity. Additionally, Sn substitution was found to reduce both electronic and lattice thermal conductivities.
In this study, tetrahedrite compounds doped with Sn were prepared by mechanical alloying and hot pressing, and their charge transport and thermoelectric properties were analyzed. X-ray diffraction analysis revealed that both the synthetic powders and sintered bodies were synthesized as a single tetrahedrite phase without secondary phases. Densely sintered specimens were obtained with relatively high densities of 99.5%-100.0% of the theoretical density, and the component elements were distributed uniformly. Sn was successfully substituted at the Sb site, and the lattice constant increased from 1.0348 to 1.0364 nm. Positive signs of the Hall and Seebeck coefficients confirmed that the Sn-doped tetrahedrites were p-type semiconductors. The carrier concentration decreased from 1.28 x 10(19) to 1.57 x 10(18) cm(-3) as the Sn content decreased because excess electrons were supplied by doping with Sn4+ at the Sb3+ site of the tetrahedrite. The Seebeck coefficient increased with increasing Sn content, and Cu12Sb3.6Sn0.4S13 exhibited maximum values of 238-270 mu VK-1 at temperatures of 323-723 K. However, the electrical conductivity decreased as the amount of Sn doping increased. Thus, Cu12Sb3.9Sn0.1S13 exhibited the highest electrical conductivity of (2.24-2.40) x 10(4) Sm-1 at temperatures of 323-723 K. A maximum power factor of 0.73 mWm(-1)K(-2) was achieved at 723 K for Cu12Sb3.9Sn0.1S13. Sn substitution reduced both the electronic and lattice thermal conductivities. The lowest thermal conductivity of 0.49-0.60 Wm(-1)K(-1) was obtained at temperatures of 323-723 K for Cu12Sb3.6Sn0.4S13, where the lattice thermal conductivity was dominant at 0.49-0.57 Wm(-1)K(-1). As a result, a maximum dimensionless figure of merit of 0.66 was achieved at 723 K for Cu12Sb3.9Sn0.1S13.
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