PbTe-based thermoelectric materials are good candidates for harvesting waste heat at mid-range temperatures due to their high thermoelectric efficiencies. Excellent quality and reliability of the bonding between the thermoelectric material and the electrode at high temperatures are essential for manufacturing thermoelectric generators. Here, a technique has been developed to achieve high-quality bonding between PbTe and the electrode. We have successfully performed one-step sintering of nickel electrode to n-type PbTe powder using spark plasma sintering. The fabricated interphase, composed of nickel telluride, is continuous and homogeneous across the junction, without visible flaws on the electrode or in the interphase and PbTe. To evaluate the long-term thermal stability of the fabricated bond, an aging test was conducted at 823 K for 360 h under vacuum. The microstructures and chemical composition of the fabricated bonding and the aged sample were investigated in detail by scanning electron microscopy equipped with energy dispersive X-ray spectroscopy analysis. No excess reaction was observed between the electrode and the thermoelectric material after aging, supporting the formation of a chemically stable interphase, which acts as a diffusion barrier. Degradation of the PbTe was detected after aging, however. The fabricated interface meets the required criteria for maximum efficiency of PbTe materials.
The efficiency of thermoelectric generators is defined by the thermoelectric performance of materials, as expressed by the thermoelectric figure-of-merit, and their contacts with electrodes. Lead chalcogenide thermoelectric materials, and in particular PbTe, perform well in the 500-900 K temperature range. Here, we have successfully bonded bulk PbTe to Ni electrode to generate a diffusion barrier, avoiding continuous reaction of the thermoelectric legs and conducting electrodes at the operating temperature. We have modified the commonly used spark plasma sintering assembly method to join Ni electrode to bulk PbTe by driving the total supplied electrical current through the Ni and PbTe solid interfaces. This permits the formation of a thin diffusion layer, roughly 4.5 µm in thickness, which is solely 2 comprised of nickel telluride. This new technique towards the bonding of PbTe with the electrode is beneficial for thermoelectric materials, since high temperatures have proven to be damaging to the quality of bulk material. The interphase microstructure, chemical composition, and crystallographic information were evaluated by a scanning electron microscope equipped with electron back-scattered diffraction analysis. The obtained phase at the Ni/PbTe contact is found to be β 2 Ni 3±x Te 2 with a basic tetragonal crystallographic structure of the defective Cu 2 Sb type.
Recently, the quaternary system PbTe-PbSe-PbS has been shown to provide high thermoelectric efficiency, zT. The intent of this research is to investigate the thermoelectric properties of Na-doped pseudoternary (PbTe) 0.65-x (PbSe) 0.35 (PbS) x with a high ratio of PbS toPbTe. The addition of a large concentration of PbSe increases the solubility limit of PbS in PbTe, allowing all samples to behave as solid solutions with a high concentration of PbS. This is proved to decrease lattice thermal conductivity due to the larger atomic mass contrast between Sulphur and Tellurium, however, simultaneously causes a decrease in the Seebeck coefficient due to a larger band offset, so a high concentration of PbS shows no improvement in zT, with a maximum of ~1.4 in the x = 0, 0.05 and 0.10 samples.
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