X-ray structural analysis and high-temperature thermoelectric properties measurements are performed on polycrystalline samples of artificial mineral Cu12−xNixSb4S13 tetrahedrite. Analysis of the atomic displacement parameter manifests low-energy vibration of Cu(2) out of CuS3 triangle plane. The vibration results in low lattice thermal conductivity of less than 0.5 W K−1 m−1. By tuning of the Ni composition x and decrease of electronic thermal conductivity, dimensionless thermoelectric figure of merit for x = 1.5 achieves 0.7 at 665 K, which is a considerably high value among p-type Pb-free sulfides. Because the tetrahedrite is an environmentally friendly material, it constitutes a good thermoelectric material for use in support of a sustainable society.
Thermoelectric technology allows conversion between heat and electricity. Many good thermoelectric materials contain rare or toxic elements, so developing low-cost and high-performance thermoelectric materials is warranted. Here, we report the temperature-dependent interplay of three separate electronic bands in hole-doped tin sulfide (SnS) crystals. This behavior leads to synergistic optimization between effective mass (m*) and carrier mobility (μ) and can be boosted through introducing selenium (Se). This enhanced the power factor from ~30 to ~53 microwatts per centimeter per square kelvin (μW cm−1 K−2 at 300 K), while lowering the thermal conductivity after Se alloying. As a result, we obtained a maximum figure of merit ZT (ZTmax) of ~1.6 at 873 K and an average ZT (ZTave) of ~1.25 at 300 to 873 K in SnS0.91Se0.09 crystals. Our strategy for band manipulation offers a different route for optimizing thermoelectric performance. The high-performance SnS crystals represent an important step toward low-cost, Earth-abundant, and environmentally friendly thermoelectrics.
High-performance thermoelectric bulk sulfide with the colusite structure is achieved by controlling the densification process and forming short-to-medium range structural defects. A simple and powerful way to adjust carrier concentration combined with enhanced phonon scattering through point defects and disordered regions is described. By combining experiments with band structure and phonons calculations, we elucidate, for the first time, the underlying mechanism at the origin of intrinsically low thermal conductivity in colusite samples as well as the effect of S vacancies and antisite defects on the carrier concentration. Our approach provides a controlled and scalable method to engineer high power factors and remarkable figures of merit near the unity in complex bulk sulfide such as CuVSnS colusites.
To grow the thermoelectric market, the module development must be at par with the advancements in the materials development. In this work, we successfully bridge the two by developing high-ZT (1.9) PbTe-based thermoelectric material and using this material in thermoelectric module development, leading to a record high efficiency of 12%. The ZT was enhanced through nanostructuring and engineered doping. The high-efficiency module will pave the way for many new opportunities for thermoelectric power generation in commercial applications.
The thermoelectric properties of crystalline melt‐grown ingots of p‐type PbTe–xMgTe (x = 1–3 mol%) doped with Na2Te (1–2 mol%) were investigated over the temperature range of 300 K to 810 K. While the powder X‐ray diffraction patterns show that all samples crystallize in the NaCl‐type structure with no MgTe or other phases present, transmission electron microscopy reveals ubiquitous MgTe nanoprecipitates in the PbTe. The very small amounts of MgTe in PbTe have only a small effect on the electrical transport properties of the system, while they have a large effect on thermal transport significantly reducing the lattice thermal conductivity. A ZT of 1.6 at 780 K is achieved for the PbTe containing 2% MgTe doped with 2% Na2Te.
We report thermoelectric (TE) properties of dense samples of colusites Cu26V2M6S32 (M = Ge, Sn), most of which are composed of earth-abundant elements; Cu and S. The combination of p-type metallic conduction and large thermopowers greater than 200 μV/K leads to high TE power factors of 0.61 and 0.48 mW/K2 m at 663 K for M = Ge and Sn samples, respectively. Furthermore, the lattice thermal conductivity is smaller than 0.6 W/Km over the temperature range from 350 K to 663 K due to the structural complexity. As a consequence, the values of dimensionless TE figure of merit ZT for M = Ge and Sn reach 0.73 and 0.56 at 663 K, respectively. Thus, the colusites are promising candidates for environmental friendly TE materials usable in the range of 500–700 K.
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