High thermoelectric performance by resonant dopant indium in nanostructured SnTe.
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ABSTRACT:
SUBMITTER: Zhang Q
PROVIDER: S-EPMC3746939 | biostudies-literature |
REPOSITORIES: biostudies-literature
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Project description:Thermoelectric materials enable the direct conversion between heat and electricity. SnTe is a promising candidate due to its high charge transport performance. Here, we prepared SnTe nanocomposites by employing an aqueous method to synthetize SnTe nanoparticles (NP), followed by a unique surface treatment prior NP consolidation. This synthetic approach allowed optimizing the charge and phonon transport synergistically. The novelty of this strategy was the use of a soluble PbS molecular complex prepared using a thiol-amine solvent mixture that upon blending is adsorbed on the SnTe NP surface. Upon consolidation with spark plasma sintering, SnTe-PbS nanocomposite is formed. The presence of PbS complexes significantly compensates for the Sn vacancy and increases the average grain size of the nanocomposite, thus improving the carrier mobility. Moreover, lattice thermal conductivity is also reduced by the Pb and S-induced mass and strain fluctuation. As a result, an enhanced ZT of ca. 0.8 is reached at 873 K. Our finding provides a novel strategy to conduct rational surface treatment on NP-based thermoelectrics.
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Project description:Lead-free chalcogenide SnTe has been demonstrated to be an efficient medium temperature thermoelectric (TE) material. However, high intrinsic Sn vacancies as well as high thermal conductivity devalue its performance. Here, ?-Zn4Sb3 is incorporated into the SnTe matrix to regulate the thermoelectric performance of SnTe. Sequential in situ reactions take place between the ?-Zn4Sb3 additive and SnTe matrix, and an interesting "core-shell" microstructure (Sb@ZnTe) is obtained; the composition of SnTe matrix is also tuned and thus Sn vacancies are compensated effectively. Benefitting from the synergistic effect of the in situ reactions, an ultralow ?lat ?0.48 W m-1 K-1 at 873 K is obtained and the carrier concentrations and electrical properties are also improved successfully. Finally, a maximum ZT ?1.32, which increases by ?220% over the pristine SnTe, is achieved in the SnTe-1.5% ?-Zn4Sb3 sample at 873 K. This work provides a new strategy to regulate the TE performance of SnTe and also offers a new insight to other related thermoelectric materials.
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Project description:SnTe has been the focus of numerous experimental and theoretical studies over the last years owing to its high thermoelectric performances near 800 K when appropriately doped. Here, we demonstrate that melt-spinning, an ultrafast-quenching synthesis technique, followed by spark plasma sintering results in enhanced ZT values in polycrystalline SnTe. To illustrate the impact of this technique, the results are contrasted with those obtained on two polycrystalline samples prepared by direct quenching of molten SnTe and without quenching. SnTe melt-spun ribbons are characterized by a peculiar columnar microstructure that contributes to lower the lattice thermal conductivity below 700 K in pressed samples. More importantly, this technique results in a significant decrease in the hole concentration, giving rise to enhanced thermopower values above 500 K. The variation in the hole concentration is likely due to a slight loss of elemental Te during the melt-spinning process. Thanks to the decreased hole concentration, the thermoelectric performances are significantly enhanced with a peak ZT value of 0.6 at 800 K, which represents a 40% increase over the values measured for samples prepared with and without quenching. These findings indicate that melt-spinning provides a novel strategy to improve the thermoelectric properties of SnTe that could be worthwhile extending to substituted compounds.
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Project description:In this study, we demonstrate the feasibility of Bi-doped tetrahedrite Cu12Sb4-xBixS13 (x = 0.02-0.20) synthesis in an industrial eccentric vibratory mill using Cu, Sb, Bi and S elemental precursors. High-energy milling was followed by spark plasma sintering. In all the samples, the prevailing content of tetrahedrite Cu12Sb4S13 (71-87%) and famatinite Cu3SbS4 (13-21%), together with small amounts of skinnerite Cu3SbS3, have been detected. The occurrence of the individual Cu-Sb-S phases and oxidation states of bismuth identified as Bi0 and Bi3+ are correlated. The most prominent effect of the simultaneous milling and doping on the thermoelectric properties is a decrease in the total thermal conductivity (κ) with increasing Bi content, in relation with the increasing amount of famatinite and skinnerite contents. The lowest value of κ was achieved for x = 0.2 (1.1 W m-1 K-1 at 675 K). However, this sample also manifests the lowest electrical conductivity σ, combined with relatively unchanged values for the Seebeck coefficient (S) compared with the un-doped sample. Overall, the lowered electrical performances outweigh the benefits from the decrease in thermal conductivity and the resulting figure-of-merit values illustrate a degradation effect of Bi doping on the thermoelectric properties of tetrahedrite in these synthesis conditions.
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Project description:The effects of doping on the transport properties of Ca5Al2Sb6 are investigated using first-principles electronic structure methods and Boltzmann transport theory. The calculated results show that a maximum ZT value of 1.45 is achieved with an optimum carrier concentration at 1000 K. However, experimental studies have shown that the maximum ZT value is no more than 1 at 1000 K. By comparing the calculated Seebeck coefficient with experimental values, we find that the low dopant solubility in this material is not conductive to achieve the optimum carrier concentration, leading a smaller experimental value of the maximum ZT. Interestingly, the calculated dopant formation energies suggest that optimum carrier concentrations can be achieved when the dopants and Sb atoms have similar electronic configurations. Therefore, it might be possible to achieve a maximum ZT value of 1.45 at 1000 K with suitable dopants. These results provide a valuable theoretical guidance for the synthesis of high-performance bulk thermoelectric materials through dopants optimization.
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