Achieving high electronic mobility and excellent thermoelectric performance in GeTe through Ge vacancy suppression and band structure engineering.

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Microstructure engineering is an effective strategy to reduce lattice thermal conductivity (κ ) and enhance the thermoelectric figure of merit (zT). Through a new process based on melt-centrifugation to squeeze out excess eutectic liquid, microstructure modulation is realized to manipulate the formation of dislocations and clean grain boundaries, resulting in a porous network with a platelet structure. In this way, phonon transport is strongly disrupted by a combination of porosity, pore surfaces/junctions, grain boundaries, and lattice dislocations. These collectively result in a ≈60% reduction of κ compared to zone melted ingot, while the charge carriers remain relatively mobile across the liquid-fused grains. This porous material displays a zT value of 1.2, which is higher than fully dense conventional zone melted ingots and hot pressed (Bi,Sb) Te alloys. A segmented leg of melt-centrifuged Bi Sb Te and Bi Sb Te could produce a high device ZT exceeding 1.0 over the whole temperature range of 323-523 K and an efficiency up to 9%. The present work demonstrates a method for synthesizing high-efficiency porous thermoelectric materials through an unconventional melt-centrifugation technique.

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Peltier devices utilizing thermoelectric (TE) materials are expected to be used for precise temperature management in 5G and next-generation communication technologies. This demand has driven efforts to develop high-TE-performance Bi2Te3-based...

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GeTe is a promising mid-temperature thermoelectric compound but inevitably contains excessive Ge vacancies hindering its performance maximization. This work reveals that significant enhancement in the dimensionless figure of merit (ZT) could be realized by defect structure engineering from point defects to line and plane defects of Ge vacancies. The evolved defects including dislocations and nanodomains enhance phonon scattering to reduce lattice thermal conductivity in GeTe. The accumulation of cationic vacancies toward the formation of dislocations and planar defects weakens the scattering against electronic carriers, securing the carrier mobility and power factor. This synergistic effect on electronic and thermal transport properties remarkably increases the quality factor. As a result, a maximum ZT > 2.3 at 648 K and a record-high average ZT (300-798 K) were obtained for Bi0.07Ge0.90Te in lead-free GeTe-based compounds. This work demonstrates an important strategy for maximizing the thermoelectric performance of GeTe-based materials by engineering the defect structures, which could also be applied to other thermoelectric materials.

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