Regulating Te Vacancies through Dopant Balancing via Excess Ag Enables Rebounding Power Factor and High Thermoelectric Performance in p-Type PbTe.

Thermoelectric properties are frequently manipulated by introducing point defects into a matrix. However, these properties often change in unfavorable directions owing to the spontaneous formation of vacancies at high temperatures. Although it is crucial to maintain high thermoelectric performance over a broad temperature range, the suppression of vacancies is challenging since their formation is thermodynamically preferred. In this study, using PbTe as a model system, it is demonstrated that a high thermoelectric dimensionless figure of merit, zT ≈ 2.1 at 723 K, can be achieved by suppressing the vacancy formation via dopant balancing. Hole-killer Te vacancies are suppressed by Ag doping because of the increased electron chemical potential. As a result, the re-dissolution of Na2 Te above 623 K can significantly increase the hole concentration and suppress the drop in the power factor. Furthermore, point defect scattering in material systems significantly reduces lattice thermal conductivity. The synergy between defect and carrier engineering offers a pathway for achieving a high thermoelectric performance by alleviating the power factor drop and can be utilized to enhance thermoelectric properties of thermoelectric materials.

Stretchable fabric generates electric power from woven thermoelectric fibers.

Assembling thermoelectric modules into fabric to harvest energy from body heat could one day power multitudinous wearable electronics. However, the invalid 2D architecture of fabric limits the application in thermoelectrics. Here, we make the valid thermoelectric fabric woven out of thermoelectric fibers producing an unobtrusive working thermoelectric module. Alternately doped carbon nanotube fibers wrapped with acrylic fibers are woven into π-type thermoelectric modules. Utilizing elasticity originating from interlocked thermoelectric modules, stretchable 3D thermoelectric generators without substrate can be made to enable sufficient alignment with the heat flow direction. The textile generator shows a peak power density of 70 mWm-2 for a temperature difference of 44 K and excellent stretchability (~80% strain) with no output degradation. The compatibility between body movement and sustained power supply is further displayed. The generators described here are true textiles, proving active thermoelectrics can be woven into various fabric architectures for sensing, energy harvesting, or thermal management.

Improvement of Low-Temperature zT in a Mg3 Sb2 -Mg3 Bi2 Solid Solution via Mg-Vapor Annealing.

Materials with high zT over a wide temperature range are essential for thermoelectric applications. n-Type Mg3 Sb2 -based compounds have been shown to achieve high zT at 700 K, but their performance at low temperatures (<500 K) is compromised due to their highly resistive grain boundaries. Syntheses and optimization processes to mitigate this grain-boundary effect has been limited due to loss of Mg, which hinders a sample's n-type dopability. A Mg-vapor anneal processing step that grows a sample's grain size and preserves its n-type carrier concentration during annealing is demonstrated. The electrical conductivity and mobility of the samples with large grain size follows a phonon-scattering-dominated T-3/2 trend over a large temperature range, further supporting the conclusion that the temperature-activated mobility in Mg3 Sb2 -based materials is caused by resistive grain boundaries. The measured Hall mobility of electrons reaches 170 cm2 V-1 s-1 in annealed 800 °C sintered Mg3 + δ Sb1.49 Bi0.5 Te0.01 , the highest ever reported for Mg3 Sb2 -based thermoelectric materials. In particular, a sample with grain size >30 mm has a zT 0.8 at 300 K, which is comparable to commercial thermoelectric materials used at room temperature (n-type Bi2 Te3 ) while reaching zT 1.4 at 700 K, allowing applications over a wider temperature scale.

Lattice Dislocations Enhancing Thermoelectric PbTe in Addition to Band Convergence.

Phonon scattering by nanostructures and point defects has become the primary strategy for minimizing the lattice thermal conductivity (κL ) in thermoelectric materials. However, these scatterers are only effective at the extremes of the phonon spectrum. Recently, it has been demonstrated that dislocations are effective at scattering the remaining mid-frequency phonons as well. In this work, by varying the concentration of Na in Pb0.97 Eu0.03 Te, it has been determined that the dominant microstructural features are point defects, lattice dislocations, and nanostructure interfaces. This study reveals that dense lattice dislocations (≈4 × 1012 cm-2 ) are particularly effective at reducing κL . When the dislocation concentration is maximized, one of the lowest κL values reported for PbTe is achieved. Furthermore, due to the band convergence of the alloyed 3% mol. EuTe the electronic performance is enhanced, and a high thermoelectric figure of merit, zT, of ≈2.2 is achieved. This work not only demonstrates the effectiveness of dense lattice dislocations as a means of lowering κL , but also the importance of engineering both thermal and electronic transport simultaneously when designing high-performance thermoelectrics.

Nanocomposites from Solution-Synthesized PbTe-BiSbTe Nanoheterostructure with Unity Figure of Merit at Low-Medium Temperatures (500-600 K).

A scalable, low-temperature solution process is used to synthesize precursor material for Pb-doped Bi0.7 Sb1.3 Te3 thermoelectric nanocomposites. The controllable Pb-doping leads to the increase in the optical bandgap, thus delaying the onset of bipolar conduction. Furthermore, the solution synthesis enables nanostructuring, which greatly reduces thermal conductivity. As a result, this material exhibits a zT = 1 over the 513-613 K range.

Ultrahigh Thermoelectric Performance in Mosaic Crystals.

Successful research strategies to enhance the dimensionless figure of merit zT above 2 rely on either bulk nanomaterials or on single crystals. A new physical mechanism of nanoscale mosaicity is shown that goes beyond the approaches in single crystals or conventional nanomaterials. A zT value of 2.1 at 1000 K in bulk nanomaterials is achieved.