Advancing Thermoelectric Performance of Bi2Te3 below 400 K.

Thermoelectric cooling devices utilizing Bi2Te3-based alloys have seen increased utilization in recent years. However, their thermoelectric performance remains inadequate within the operational temperature range (≤400 K), with limited research addressing this issue. In this study, we successfully modulated the carrier concentration of the sample through Te content reduction, consequently lowering the peak temperature of the zT value from 400 to 300 K. This led to a substantial enhancement in thermoelectric performance at room temperature (≤400 K). Furthermore, by doping with La, the electrical transport properties have been further optimized, and the lattice thermal conductivity has been effectively reduced at the same time; the average zT value was ultimately elevated from 0.69 to 0.9 within the temperature range of 300-400 K. These findings hold significant promise for enhancing the efficacy of existing thermoelectric cooling devices based on Bi2Te3-based alloys.

Robustly Enhanced Seebeck Coefficient in the MXene/Organics/TiS2 Misfit Structure for Flexible Thermoelectrics.

The flexible thermoelectric (TE) generator has emerged as a superior alternative to traditional batteries for powering wearable electronic devices, as it can efficiently convert skin heat into electricity without any safety concerns. MXene, a highly researched two-dimensional material, is known for its exceptional flexibility, hydrophilicity, metallic conductivity, and processability, among other properties, making it a versatile material for a wide range of applications, including supercapacitors, electromagnetic shielding, and sensors. However, the low intrinsic Seebeck coefficient of MXene due to its metallic conducting nature poses a significant challenge to its TE application. Therefore, improving the Seebeck coefficient remains a primary concern. In this regard, a flexible MXene/organics/TiS2 misfit film was synthesized in this work through organic intercalation, exfoliation, and re-assembly techniques. The absolute value of Seebeck coefficient of the misfit film was significantly enhanced to 44.8 µV K-1, which is five times higher than that of the original MXene film. This enhancement is attributed primarily to the weighted effect of the Seebeck coefficient and possibly to energy-filtering effects at the heterogeneous interfaces. Additionally, the power factor of the misfit film was considerably improved to 77.2 µW m-1 K-2, which is 18 times higher than that of the original MXene film. The maximum output power of the TE device constructed of the misfit film was 95 nW at a temperature difference of 40 K, resulting in a power density of 1.18 W m-2, demonstrating the significant potential of this technology for driving low-energy consumption wearable electronics.

A Bi2Te3-Filled Nickel Foam Film with Exceptional Flexibility and Thermoelectric Performance.

The past decades have witnessed surging demand for wearable electronics, for which thermoelectrics (TEs) are considered a promising self-charging technology, as they are capable of converting skin heat into electricity directly. Bi2Te3 is the most-used TE material at room temperature, due to a high zT of ~1. However, it is different to integrate Bi2Te3 for wearable TEs owing to its intrinsic rigidity. Bi2Te3 could be flexible when made thin enough, but this implies a small electrical and thermal load, thus severely restricting the power output. Herein, we developed a Bi2Te3/nickel foam (NiFoam) composite film through solvothermal deposition of Bi2Te3 nanoplates into porous NiFoam. Due to the mesh structure and ductility of Ni Foam, the film, with a thickness of 160 µm, exhibited a high figure of merit for flexibility, 0.016, connoting higher output. Moreover, the film also revealed a high tensile strength of 12.7 ± 0.04 MPa and a maximum elongation rate of 28.8%. In addition, due to the film's high electrical conductivity and enhanced Seebeck coefficient, an outstanding power factor of 850 µW m-1 K-2 was achieved, which is among the highest ever reported. A module fabricated with five such n-type legs integrated electrically in series and thermally in parallel showed an output power of 22.8 nW at a temperature gap of 30 K. This work offered a cost-effective avenue for making highly flexible TE films for power supply of wearable electronics by intercalating TE nanoplates into porous and meshed-structure materials.

Ultra-dense dislocations stabilized in high entropy oxide ceramics.

Dislocations are commonly present and important in metals but their effects have not been fully recognized in oxide ceramics. The large strain energy raised by the rigid ionic/covalent bonding in oxide ceramics leads to dislocations with low density (∼106 mm-2), thermodynamic instability and spatial inhomogeneity. In this paper, we report ultrahigh density (∼109 mm-2) of edge dislocations that are uniformly distributed in oxide ceramics with large compositional complexity. We demonstrate the dislocations are progressively and thermodynamically stabilized with increasing complexity of the composition, in which the entropy gain can compensate the strain energy of dislocations. We also find cracks are deflected and bridged with ∼70% enhancement of fracture toughness in the pyrochlore ceramics with multiple valence cations, due to the interaction with enlarged strain field around the immobile dislocations. This research provides a controllable approach to establish ultra-dense dislocations in oxide ceramics, which may open up another dimension to tune their properties.

Enhanced thermoelectric performance in polymorphic heavily Co-doped Cu2SnS3 through carrier compensation by Sb substitution.

Heavily acceptor-doped Cu2SnS3 (CTS) shows promisingly large power factor (PF) due to its rather high electrical conductivity (σ) which causes a modest ZT with a high electronic thermal conductivity (κe ). In the present work, a strategy of carrier compensation through Sb-doping at the Sn site in Cu2Sn0.8Co0.2S3 was investigated, aiming at tailoring electrical and phonon transport properties simultaneously. Rietveld analysis suggested a complex polymorphic microstructure in which the cation-(semi)ordered tetragonal phase becomes dominant over the coherently bonded cation-disordered cubic phase, as is preliminarily revealed using TEM observation, upon Sb-doping and Sb would substitute Sn preferentially in the tetragonal structure. With increasing content of Sb, the σ was lowered and the Seebeck coefficient (S) was enhanced effectively, which gave rise to high PFs maintained at ~10.4 µWcm-1K-2 at 773 K together with an optimal reduction in κe by 60-70% in the whole temperature range. The lattice thermal conductivity was effectively suppressed from 1.75 Wm-1K-1 to ~1.2 Wm-1K-1 at 323 K while maintained very low at 0.3-0.4 Wm-1K-1 at 773 K. As a result, a peak ZT of ~0.88 at 773 K has been achieved for Cu2Sn0.74Sb0.06Co0.2S3, which stands among the tops so far of the CTS-based diamond-like ternary sulfides. These findings demonstrate that polymorphic microstructures with cation-disordered interfaces as an approach to achieve effective phonon-blocking and low lattice thermal conductivity, of which further crystal chemistry, microstructural and electrical tailoring are possible by appropriate doping.

Embedding two-dimensional graphene array in ceramic matrix.

Dispersing two-dimensional (2D) graphene sheets in 3D material matrix becomes a promising route to access the exceptional mechanical and electrical properties of individual graphene sheets in bulk quantities for macroscopic applications. However, this is highly restricted by the uncontrolled distribution and orientation of the graphene sheets in 3D structures as well as the weak graphene-matrix bonding and poor load transfer. Here, we propose a previously unreported avenue to embed ordered 2D graphene array into ceramics matrix, where the catastrophic fracture failure mode of brittle ceramics was transformed into stable crack propagation behavior with 250 to 500% improvement in the mechanical toughness. An unprecedentedly low dry sliding friction coefficient of 0.06 in bulk ceramics was obtained mainly due to the inhibition of the microcrack propagation by the ordered 2D graphene array. These unique and low-cost 2D graphene array/ceramic composites may find applications in severe environments with superior structural and functional properties.

Flexible Foil of Hybrid TaS2 /Organic Superlattice: Fabrication and Electrical Properties.

TaS2 nanolayers with reduced dimensionality show interesting physics, such as a gate-tunable phase transition and enhanced superconductivity, among others. Here, a solution-based strategy to fabricate a large-area foil of hybrid TaS2 /organic superlattice, where [TaS2 ] monolayers and organic molecules alternatively stack in atomic scale, is proposed. The [TaS2 ] layers are spatially isolated with remarkably weakened interlayer bonding, resulting in lattice vibration close to that of TaS2 monolayers. The foil also shows excellent mechanical flexibility together with a large electrical conductivity of 1.2 × 103 S cm-1 and an electromagnetic interference of 31 dB, among the highest values for solution-processed thin films of graphene and inorganic graphene analogs. The solution-based strategy reported herein can add a new dimension to manipulate the structure and properties of 2D materials and provide new opportunities for flexible nanoelectronic devices.