Search

High thermoelectric performance is generally achieved through either electronic structure modulations or phonon scattering enhancements, which often counteract each other. A leap in performance requires innovative strategies that simultaneously optimize electronic and phonon transports. We demonstrate high thermoelectric performance with a near room-temperature figure of merit, ZT ~ 1.5, and a maximum ZT ~ 2.6 at 573 kelvin, by optimizing atomic disorder in cadmium-doped polycrystalline silver antimony telluride (AgSbTe2). Cadmium doping in AgSbTe2 enhances cationic ordering, which simultaneously improves electronic properties by tuning disorder-induced localization of electronic states and reduces lattice thermal conductivity through spontaneous formation of nanoscale (~2 to 4 nanometers) superstructures and coupling of soft vibrations localized within ~1 nanometer around cadmium sites with local strain modulation. The strategy is applicable to most other thermoelectric materials that exhibit inherent atomic disorder. [ABSTRACT FROM AUTHOR]

The realization of n‐type Ge chalcogenides is elusive owing to intrinsic Ge vacancies that make them p‐type semiconductors. GeSe crystallizes into a layered orthorhombic structure similar to SnSe at ambient conditions. The high‐symmetry cubic phase of GeSe is predicted to be stabilized by applying 7 GPa external pressure or by enhancing the entropy by increasing to temperature to 920 K. Stabilization of the n‐type cubic phase of GeSe at ambient conditions was achieved by alloying with AgBiSe2 (30–50 mol %), enhancing the entropy through solid solution mixing. The interplay of positive and negative chemical pressure anomalously changes the band gap of GeSe with increasing the AgBiSe2 concentration. The band gap of n‐type cubic (GeSe)1−x(AgBiSe2)x (0.30≤x≤0.50) has a value in the 0.3–0.4 eV range, which is significantly lower than orthorhombic GeSe (1.1 eV). Cubic (GeSe)1−x(AgBiSe2)x exhibits an ultralow lattice thermal conductivity (κL≈0.43 W m−1 K−1) in the 300–723 K range. The low κL is attributed to significant phonon scattering by entropy‐driven enhanced solid‐solution point defects. [ABSTRACT FROM AUTHOR]

Abstract: Crystalline solids with intrinsically low lattice thermal conductivity (κL) are crucial to realizing high‐performance thermoelectric (TE) materials. Herein, we show an ultralow κL of 0.35 Wm−1 K−1 in AgCuTe, which has a remarkable TE figure‐of‐merit, zT of 1.6 at 670 K when alloyed with 10 mol % Se. First‐principles DFT calculation reveals several soft phonon modes in its room‐temperature hexagonal phase, which are also evident from low‐temperature heat‐capacity measurement. These phonon modes, dominated by Ag vibrations, soften further with temperature giving a dynamic cation disorder and driving the superionic transition. Intrinsic factors cause an ultralow κL in the room‐temperature hexagonal phase, while the dynamic disorder of Ag/Cu cations leads to reduced phonon frequencies and mean free paths in the high‐temperature rocksalt phase. Despite the cation disorder at elevated temperatures, the crystalline conduits of the rigid anion sublattice give a high power factor. [ABSTRACT FROM AUTHOR]

Waste heat sources are generally diffused and provide a range of temperatures rather than a particular temperature. Thus, thermoelectric waste heat to electricity conversion requires a high average thermoelectric figure of merit ( ZTavg) of materials over the entire working temperature along with a high peak thermoelectric figure of merit ( ZTmax). Herein an ultrahigh ZTavg of 1.4 for (GeTe)80(AgSbSe2)20 [TAGSSe-80, T=tellurium, A=antimony, G=germanium, S=silver, Se=selenium] is reported in the temperature range of 300-700 K, which is one of the highest values measured amongst the state-of-the-art Pb-free polycrystalline thermoelectric materials. Moreover, TAGSSe-80 exhibits a high ZTmax of 1.9 at 660 K, which is reversible and reproducible with respect to several heating-cooling cycles. The high thermoelectric performance of TAGSSe- x is attributed to extremely low lattice thermal conductivity ( κlat), which mainly arises due to extensive phonon scattering by hierarchical nano/meso-structures in the TAGSSe- x matrix. Addition of AgSbSe2 in GeTe results in κlat of ≈0.4 W mK−1 in the 300-700 K range, approaching to the theoretical minimum limit of lattice thermal conductivity ( κmin) of GeTe. Additionally, (GeTe)80(AgSbSe2)20 exhibits a higher Vickers microhardness (mechanical stability) value of ≈209 kgf mm−2 compared to the other state-of-the-art metal chalcogenides, making it an important material for thermoelectrics. [ABSTRACT FROM AUTHOR]

Waste heat sources are generally diffused and provide a range of temperatures rather than a particular temperature. Thus, thermoelectric waste heat to electricity conversion requires a high average thermoelectric figure of merit ( ZTavg) of materials over the entire working temperature along with a high peak thermoelectric figure of merit ( ZTmax). Herein an ultrahigh ZTavg of 1.4 for (GeTe)80(AgSbSe2)20 [TAGSSe-80, T=tellurium, A=antimony, G=germanium, S=silver, Se=selenium] is reported in the temperature range of 300-700 K, which is one of the highest values measured amongst the state-of-the-art Pb-free polycrystalline thermoelectric materials. Moreover, TAGSSe-80 exhibits a high ZTmax of 1.9 at 660 K, which is reversible and reproducible with respect to several heating-cooling cycles. The high thermoelectric performance of TAGSSe- x is attributed to extremely low lattice thermal conductivity ( κlat), which mainly arises due to extensive phonon scattering by hierarchical nano/meso-structures in the TAGSSe- x matrix. Addition of AgSbSe2 in GeTe results in κlat of ≈0.4 W mK−1 in the 300-700 K range, approaching to the theoretical minimum limit of lattice thermal conductivity ( κmin) of GeTe. Additionally, (GeTe)80(AgSbSe2)20 exhibits a higher Vickers microhardness (mechanical stability) value of ≈209 kgf mm−2 compared to the other state-of-the-art metal chalcogenides, making it an important material for thermoelectrics. [ABSTRACT FROM AUTHOR]

Topological crystalline insulator (TCI), Pb0.6Sn0.4Te, exhibits metallic surface states protected by crystal mirror symmetry with negligibly small band gap. Enhancement of its thermoelectric performances needs tuning of its electronic structure particularly through engineering of its band gap. While physical perturbations tune the electronic structure of TCI by breaking of the crystal mirror symmetry, chemical means such as doping have been more attractive recently as they result in better thermoelectric performance in TCIs. Here, we demonstrate that K doping in TCI, Pb0.6Sn0.4Te, breaks the crystal mirror symmetry locally and widens electronic band gap, which is confirmed by direct electronic absorption spectroscopy and electronic structure calculations. K doping in Pb0.6Sn0.4Te increases p-type carrier concentration and suppresses the bipolar conduction via widening a band gap, which collectively boosts the thermoelectric figure of merit (ZT) to 1 at 708K. [ABSTRACT FROM AUTHOR]

Ge1-xSbxTe (x = 0-0.1) is prepared from the elements (evacuated quartz tubes, 1223 K, 6 h). [ABSTRACT FROM AUTHOR]