Selective Dissolution-Derived Nanoporous Design of Impurity-Free Bi2 Te3 Alloys with High Thermoelectric Performance.

Thermoelectric technology, which has been receiving attention as a sustainable energy source, has limited applications because of its relatively low conversion efficiency. To broaden their application scope, thermoelectric materials require a high dimensionless figure of merit (ZT). Porous structuring of a thermoelectric material is a promising approach to enhance ZT by reducing its thermal conductivity. However, nanopores do not form in thermoelectric materials in a straightforward manner; impurities are also likely to be present in thermoelectric materials. Here, a simple but effective way to synthesize impurity-free nanoporous Bi0.4 Sb1.6 Te3 via the use of nanoporous raw powder, which is scalably formed by the selective dissolution of KCl after collision between Bi0.4 Sb1.6 Te3 and KCl powders, is proposed. This approach creates abundant nanopores, which effectively scatter phonons, thereby reducing the lattice thermal conductivity by 33% from 0.55 to 0.37 W m-1 K-1 . Benefitting from the optimized porous structure, porous Bi0.4 Sb1.6 Te3 achieves a high ZT of 1.41 in the temperature range of 333-373 K, and an excellent average ZT of 1.34 over a wide temperature range of 298-473 K. This study provides a facile and scalable method for developing high thermoelectric performance Bi2 Te3 -based alloys that can be further applied to other thermoelectric materials.

Growth and thermoelectric properties of multilayer thin film of bismuth telluride and indium selenide via rf magnetron sputtering.

A bismuth telluride (BT)/indium selenide (IS) multilayer film was deposited at room temperature by rf magnetron sputtering on a sapphire substrate in order to investigate how the multilayered structure affects the microstructure and thermoelectric properties. The effect of annealing at different temperatures was also studied. The results were compared with those from a BT film with the same thickness. A TEM study showed that the interface between the BT and IS layers became vague as the annealing temperature increased, and the BT layer crystallized while the IS layer did not. The presence of thin IS layers can help to limit the evaporation of Te from the BT/IS multilayer film, thus increasing the amount of Bi2Te3 phase in the multilayer film as compared with that of the BT film. An abrupt increase in the Seebeck coefficient of the multilayer film was observed when annealed at 300 degrees C, and the resistivity of the annealed multilayer film was high compared to that of the BT film. This result can also be explained by the proposed role of the IS layer, which limits the evaporation of Te at high temperature. The highest power factor of -3.9 x 10(-6) W/K2 cm was obtained at room temperature from the multilayer film annealed at 300 degrees C.

Thermoelectric properties of Bi2Te3-In2Se3 composite thin films prepared by co-sputtering.

Bi2Te3-In2Se3 films were prepared by co-sputtering followed by annealing, and their structural and thermoelectric properties were investigated. The immiscible nature of the two alloys results in precipitation of the second phase, thus leading to structures with self-assembled dots that are a few nanometers in scale. HAADF-STEM and HRTEM were used to confirm that In2Se3 nanodots that were a few nanometers in size did indeed form in the Bi2Te3 thin film. It was found that the incorporation of these nanodots can reduce the thermal conductivity of the thin film.

Operation of Wearable Thermoelectric Generators Using Dual Sources of Heat and Light.

A wearable thermoelectric generator (WTEG) that utilizes human body heat can be a promising candidate for the wearable power generators. The temperature difference (ΔT) between the body and the environment is a stable source driving the WTEG, but this driving force is limited by the ambient temperature itself at the same time. Here, a novel WTEG that can be operated using the dual source of body heat and light with exceptionally high driving force is fabricated. The printable solar absorbing layer attached to the bottom of the WTEG absorbs ≈95% of the light from ultraviolet to far infrared and converts it into heat. To optimize the power density of WTEGs, the fill factor of the thermoelectric (TE) leg/electrode is considered through finite-difference time-domain (FDTD) simulation. When operated by the dual sources, the WTEG exhibits a power density of 15.33 µW cm-2 , which is the highest under "actual operating conditions" among all kinds of WTEGs. In addition, unlike conventional WTEGs, the WTEG retains 83.1% of its output power at an ambient temperature of 35 °C compared to its output power at room temperature. This study will accelerate the commercialization of WTEGs by introducing a novel method to overcome their limitations.

Precision Interface Engineering of an Atomic Layer in Bulk Bi2Te3 Alloys for High Thermoelectric Performance.

Grafting nanotechnology on thermoelectric materials leads to significant advances in their performance. Creation of structural defects including nano-inclusion and interfaces via nanostructuring achieves higher thermoelectric efficiencies. However, it is still challenging to optimize the nanostructure via conventional fabrication techniques. The thermal instability of nanostructures remains an issue in the reproducibility of fabrication processes and long-term stability during operation. This work presents a versatile strategy to create numerous interfaces in a thermoelectric material via an atomic-layer deposition (ALD) technique. An extremely thin ZnO layer was conformally formed via ALD over the Bi0.4Sb1.6Te3 powders, and numerous heterogeneous interfaces were generated from the formation of Bi0.4Sb1.6Te3-ZnO core-shell structures even after high-temperature sintering. The incorporation of ALD-grown ZnO into the Bi0.4Sb1.6Te3 matrix blocks phonon propagation and also provides tunability in electronic carrier density via impurity doping at the heterogeneous grain boundaries. The exquisite control in the ALD cycles provides a high thermoelectric performance of zT = 1.50 ± 0.15 (at 329-360 K). Specifically, ALD is an industry compatible technique that allows uniform and conformal coating over large quantities of powders. The study is promising in terms of the mass production of nanostructured thermoelectric materials with considerable improvements in performance via an industry compatible and reproducible route.

Free-electron creation at the 60° twin boundary in Bi2Te3.

Interfaces, such as grain boundaries in a solid material, are excellent regions to explore novel properties that emerge as the result of local symmetry-breaking. For instance, at the interface of a layered-chalcogenide material, the potential reconfiguration of the atoms at the boundaries can lead to a significant modification of the electronic properties because of their complex atomic bonding structure. Here, we report the experimental observation of an electron source at 60° twin boundaries in Bi2Te3, a representative layered-chalcogenide material. First-principles calculations reveal that the modification of the interatomic distance at the 60° twin boundary to accommodate structural misfits can alter the electronic structure of Bi2Te3. The change in the electronic structure generates occupied states within the original bandgap in a favourable condition to create carriers and enlarges the density-of-states near the conduction band minimum. The present work provides insight into the various transport behaviours of thermoelectrics and topological insulators.

High mobility, large linear magnetoresistance, and quantum transport phenomena in Bi2Te3 films grown by metallo-organic chemical vapor deposition (MOCVD).

We investigated the magnetotransport properties of Bi2Te3 films grown on GaAs (001) substrate by a cost-effective metallo-organic chemical vapor deposition (MOCVD). We observed the remarkably high carrier mobility and the giant linear magnetoresistance (carrier mobility ∼ 22 000 cm(2) V(-1) s(-1), magnetoresistance ∼ 750% at 1.8 K and 9 T for a 100 nm thick film) that depends on the film thickness. In addition, the Shubnikov-de Haas oscillation was observed, from which the effective mass was calculated to be consistent with the known value. From the thickness dependence of the Shubnikov-de Haas oscillation, it was found that a two dimensional electron gas with the conventional electron nature coexists with the topological Dirac fermion states and dominates the carrier transport in the Bi2Te3 film with thickness higher than 300 nm. These results are attributed to the intrinsic nature of Bi2Te3 in the high-mobility transport regime obtained by a deliberate choice of the substrate and the growth conditions.