Research in stretchable conductors is fuelled by diverse technological needs. Flexible electronics, neuroprosthetic and cardiostimulating implants, soft robotics and other curvilinear systems require materials with high conductivity over a tensile strain of 100 per cent (refs 1-3). Furthermore, implantable devices or stretchable displays need materials with conductivities a thousand times higher while retaining a strain of 100 per cent. However, the molecular mechanisms that operate during material deformation and stiffening make stretchability and conductivity fundamentally difficult properties to combine. The macroscale stretching of solids elongates chemical bonds, leading to the reduced overlap and delocalization of electronic orbitals. This conductivity-stretchability dilemma can be exemplified by liquid metals, in which conduction pathways are retained on large deformation but weak interatomic bonds lead to compromised strength. The best-known stretchable conductors use polymer matrices containing percolated networks of high-aspect-ratio nanometre-scale tubes or nanowires to address this dilemma to some extent. Further improvements have been achieved by using fillers (the conductive component) with increased aspect ratio, of all-metallic composition, or with specific alignment (the way the fillers are arranged in the matrix). However, the synthesis and separation of high-aspect-ratio fillers is challenging, stiffness increases with the volume content of metallic filler, and anisotropy increases with alignment. Pre-strained substrates, buckled microwires and three-dimensional microfluidic polymer networks have also been explored. Here we demonstrate stretchable conductors of polyurethane containing spherical nanoparticles deposited by either layer-by-layer assembly or vacuum-assisted flocculation. High conductivity and stretchability were observed in both composites despite the minimal aspect ratio of the nanoparticles. These materials also demonstrate the electronic tunability of mechanical properties, which arise from the dynamic self-organization of the nanoparticles under stress. A modified percolation theory incorporating the self-assembly behaviour of nanoparticles gave an excellent match with the experimental data.
In this study, a series of GeMnTe (x = 0-0.21) compounds were prepared by a melting-quenching-annealing process combined with spark plasma sintering (SPS). The effect of alloying MnTe into GeTe on the structure and thermoelectric properties of GeMnTe is profound. With increasing content of MnTe, the structure of the GeMnTe compounds gradually changes from rhombohedral to cubic, and the known R3m to Fm-3m phase transition temperature of GeTe moves from 700 K closer to room temperature. First-principles density functional theory calculations show that alloying MnTe into GeTe decreases the energy difference between the light and heavy valence bands in both the R3m and Fm-3m structures, enhancing a multiband character of the valence band edge that increases the hole carrier effective mass. The effect of this band convergence is a significant enhancement in the carrier effective mass from 1.44 m (GeTe) to 6.15 m (GeMnTe). In addition, alloying with MnTe decreases the phonon relaxation time by enhancing alloy scattering, reduces the phonon velocity, and increases Ge vacancies all of which result in an ultralow lattice thermal conductivity of 0.13 W m K at 823 K. Subsequent doping of the GeMnTe compositions with Sb lowers the typical very high hole carrier concentration and brings it closer to its optimal value enhancing the power factor, which combined with the ultralow thermal conductivity yields a maximum ZT value of 1.61 at 823 K (for GeMnSbTe). The average ZT value of the compound over the temperature range 400-800 K is 1.09, making it the best GeTe-based thermoelectric material.
Bismuth telluride based thermoelectric materials have been commercialized for a wide range of applications in power generation and refrigeration. However, the poor machinability and susceptibility to brittle fracturing of commercial ingots often impose significant limitations on the manufacturing process and durability of thermoelectric devices. In this study, melt spinning combined with a plasma‐activated sintering (MS‐PAS) method is employed for commercial p‐type zone‐melted (ZM) ingots of Bi0.5Sb1.5Te3. This fast synthesis approach achieves hierarchical structures and in‐situ nanoscale precipitates, resulting in the simultaneous improvement of the thermoelectric performance and the mechanical properties. Benefitting from a strong suppression of the lattice thermal conductivity, a peak ZT of 1.22 is achieved at 340 K in MS‐PAS synthesized structures, representing about a 40% enhancement over that of ZM ingots. Moreover, MS‐PAS specimens with hierarchical structures exhibit superior machinability and mechanical properties with an almost 30% enhancement in their fracture toughness, combined with an eightfold and a factor of six increase in the compressive and flexural strength, respectively. Accompanied by an excellent thermal stability up to 200 °C for the MS‐PAS synthesized samples, the MS‐PAS technique demonstrates great potential for mass production and large‐scale applications of Bi2Te3 related thermoelectrics.
High performance BiSbTe alloy and modules with a conversion efficiency of 5% are achieved through integrating Zn induced defect complexity with nanostructuring.
Large reductions in the thermal conductivity of thermoelectrics using nanostructures have been widely demonstrated. Some enhancements in the thermopower through nanostructuring have also been reported. However, these improvements are generally offset by large drops in the electrical conductivity due to a drastic reduction in the mobility. Here, we show that large enhancements in the thermopower and electrical conductivity of half-Heusler (HH) phases can be achieved simultaneously at high temperatures through coherent insertion of nanometer scale full-Heusler (FH) inclusions within the matrix. The enhancements in the thermopower of the HH/FH nanocomposites arise from drastic reductions in the "effective" carrier concentration around 300 K. Surprisingly, the mobility increases drastically, which compensates for the decrease in the carrier concentration and minimizes the drop in the electrical conductivity. Interestingly, the carrier concentration in HH/FH nanocomposites increases rapidly with temperature, matching that of the HH matrix at high temperatures, whereas the temperature dependence of the mobility significantly deviates from the typical T(-α) law and slowly decreases (linearly) with rising temperature. This remarkable interplay between the temperature dependence of the carrier concentration and mobility in the nanocomposites results in large increases in the power factor at 775 K. In addition, the embedded FH nanostructures also induce moderate reductions in the thermal conductivity leading to drastic increases in the ZT of HH(1 - x)/FH(x) nanocomposites at 775 K. By combining transmission electron microscopy and charge transport data, we propose a possible charge carrier scattering mechanism at the HH/FH interfaces leading to the observed anomalous electronic transport in the synthesized HH(1 - x)/FH(x) nanocomposites.
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