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Porous thermoelectric materials offer exciting prospects for improving the thermoelectric performance by significantly reducing the thermal conductivity. Nevertheless, porous structures are affected by issues, including restricted enhancements in performance attributed to decreased electronic conductivity and degraded mechanical strength. This study introduces an innovative strategy for overcoming these challenges using porous Bi0.4Sb1.6Te3 (BST) by combining porous structuring and interface engineering via atomic layer deposition (ALD). Porous BST powder was produced by selectively dissolving KCl in a milled mixture of BST and KCl; the interfaces were engineered by coating ZnO films through ALD. This novel architecture remarkably reduced the thermal conductivity owing to the presence of several nanopores and ZnO/BST heterointerfaces, promoting efficient phonon scattering. Additionally, the ZnO coating mitigated the high resistivity associated with the porous structure, resulting in an improved power factor. Consequently, the ZnO-coated porous BST demonstrated a remarkable enhancement in thermoelectric efficiency, with a maximum zT of approximately 1.53 in the temperature range of 333-353 K, and a zT of 1.44 at 298 K. Furthermore, this approach plays a significant role in enhancing the mechanical strength, effectively mitigating a critical limitation of porous structures. These findings open new avenues for the development of advanced porous thermoelectric materials and highlight their potential for precise interface engineering through the ALD.
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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.
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This article explores the deep learning approach towards approximating the effective electrical and thermal conductivities of copper (Cu)-carbon nanotube (CNT) composites with CNTs aligned to the field direction. Convolutional neural networks (CNN) are trained to map the two-dimensional images of stochastic Cu-CNT networks to corresponding conductivities. The CNN model learns to estimate the Cu-CNT composite conductivities for various CNT volume fractions, interfacial electrical resistances, Rc = 20 Ω-20 kΩ, and interfacial thermal resistances, Râ³t,c = 10-10-10-7 m2K/W. For training the CNNs, the hyperparameters such as learning rate, minibatch size, and hidden layer neurons are optimized. Without iteratively solving the physical governing equations, the trained CNN model approximates the electrical and thermal conductivities within a second with the coefficient of determination (R2) greater than 98%, which may take longer than 100 min for a convectional numerical simulation. This work demonstrates the potential of the deep learning surrogate model for the complex transport processes in composite materials.
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Nanotubos de Carbono , Simulación por Computador , Conductividad Eléctrica , Redes Neurales de la Computación , Conductividad TérmicaRESUMEN
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.
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Calor , Dispositivos Electrónicos Vestibles , Suministros de Energía Eléctrica , Electrodos , Humanos , Luz SolarRESUMEN
As power-conversion devices, flexible thermoelectrics that enable conformal contact with heat sources of arbitrary shape are attractive. However, the low performance of flexible thermoelectric materials, which does not exceed those of brittle inorganic counterparts, hampers their practical applications. Herein, we propose inorganic chalcogenide-nanostructured carbon nanotube (CNT) yarns with outstanding power factor at a low temperature using electrochemical deposition. The inorganic chalcogenide-nanostructured CNT yarns exhibit the power factors of 3425 and 2730 µW/(m·K2) at 298 K for the p- and n-type, respectively, which is higher than those of previously reported flexible TE materials. On the basis of excellent performance and geometry advantage of the nanostructured CNT yarn for modular design, all-CNT based thermoelectric generators have been easily fabricated, showing the maximum power densities of 24 and 380 mW/m2 at ΔT = 5 and 20 K, respectively. These results provide a promising strategy for the realization of high-performance flexible thermoelectric materials and devices for flexible/or wearable self-powering systems.
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Softening of thermoelectric generators facilitates conformal contact with arbitrary-shaped heat sources, which offers an opportunity to realize self-powered wearable applications. However, existing wearable thermoelectric devices inevitably exhibit reduced thermoelectric conversion efficiency due to the parasitic heat loss in high-thermal-impedance polymer substrates and poor thermal contact arising from rigid interconnects. Here, we propose compliant thermoelectric generators with intrinsically stretchable interconnects and soft heat conductors that achieve high thermoelectric performance and unprecedented conformability simultaneously. The silver-nanowire-based soft electrodes interconnect bismuth-telluride-based thermoelectric legs, effectively absorbing strain energy, which allows our thermoelectric generators to conform perfectly to curved surfaces. Metal particles magnetically self-assembled in elastomeric substrates form soft heat conductors that significantly enhance the heat transfer to the thermoelectric legs, thereby maximizing energy conversion efficiency on three-dimensional heat sources. Moreover, automated additive manufacturing paves the way for realizing self-powered wearable applications comprising hundreds of thermoelectric legs with high customizability under ambient conditions.
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Two-dimensional (2D) metal dichalcogenides have drawn considerable interest because they offer possibilities for the implementation of emerging electronics. The emerging electronics are moving toward two major directions: vertical expansion of device space and flexibility. However, the development of a synthesis method for 2D metal dichalcogenides that meets all the requirements remains a significant challenge. Here, we propose a promising method for wafer-scale, conformal, and low-temperature (≤240 °C) synthesis of single-phase SnS2 via the atomic layer deposition technique. There is a trade-off relationship between the crystallinity and orientation preference of SnS2, which is efficiently eliminated by the two-step growth occurring at different temperatures. Consequently, the van der Waals layers of the highly crystalline SnS2 are parallel to the substrate. Thin-film transistors (TFTs) comprising the SnS2 layer show reasonable electrical performances (field-effect mobility: â¼0.8 cm2 V-1 s-1 and on/off ratio: â¼106), which are comparable to that of a single-crystal SnS2 flake. Moreover, we demonstrate nonplanar and flexible TFTs to identify the feasibility of the implementation of future electronics. Both the diagonal-structured TFT and flexible TFT fabricated without a transfer process show electrical performances comparable to those of rigid and planar TFTs. Particularly, the flexible TFT does not exhibit substantial degradation even after 2000 bending cycles. Our work would provide decisive opportunities for the implementation of future electronic devices utilizing 2D metal chalcogenides.
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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.
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Research on two-dimensional (2D) metal dichalcogenides is rapidly expanding owing to their unique characteristics that do not exist in bulk materials. The industrially compatible development of these emerging materials is indispensable to facilitate the transition of 2D metal dichalcogenides from the research stage to the practical industrial application stage. However, an industrially relevant method, i.e., the low-temperature synthesis of wafer-scale, continuous, and orientation-controlled 2D metal dichalcogenides, still remains a significant challenge. Here, we report the low-temperature (≤350 °C) synthesis of uniform and continuous n-type SnS2 thin films via the combination of atomic layer deposition (ALD) of tin oxides and subsequent sulfurization. Well-crystallized and aligned SnS2 layers parallel to the substrate are demonstrated through the phase engineering of the ALD-grown tin oxide and the substrate surface. The additional H2S plasma treatment at 300 °C leads to the formation of stoichiometric SnS2. The formation of conformal SnS2 layers over a three-dimensional undulating hole structure is confirmed, which reveals the potential for applications beyond the planar structured architecture. The present results could be a step toward the realization of 2D metal dichalcogenides in industry.
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Despite the wide applicability of oxynitrides from photocatalysis to refractory coatings, our understanding of the materials has been limited in terms of their thermodynamics. The configurational entropy via randomly mixed O/N or via cation vacancies are known to stabilize oxynitrides, despite the positive formation enthalpies. Here, using tin oxynitrides as a model system, we show by ab initio computations that oxynitrides in seemingly charge-unbalanced composition stabilize by forming pernitrides among metal-(O,N)6 octahedra. The nitrogen pernitride dimer, =(N-N)=, results in the effective charge of -4, facilitating the formation of nitrogen-rich oxynitrides. We report that the dimer forms only in structures with corner-sharing octahedra, since the N-N bond formation requires sufficient rotational degrees of freedom among the octahedra. X-ray photoemission spectra of the synthesized tin oxynitride films reveal two distinct nitrogen bonding environments, confirming the computation results. This work opens the search space for a novel kind of oxynitrides stabilized by N dimer formation, with specific structural selection rules.
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Rutile TiO2, a high temperature phase, has attracted interest as a capacitor dielectric in dynamic random-access memories (DRAMs). Despite its high dielectric constant of >80, large leakage currents caused by a low Schottky barrier height at the TiO2/electrode interface have hindered the use of rutile TiO2 as a commercial DRAM capacitor. Here, we propose a new Ru-Pt alloy electrode to increase the height of the Schottky barrier. The Ru-Pt mixed layer was grown by atomic layer deposition. The atomic ratio of Ru/Pt varied in the entire range from 100 at.% Ru to 100 at.% Pt. Rutile TiO2 films were inductively formed only on the Ru-Pt layer containing ≤43 at.% Pt, while anatase TiO2 films with a relatively low dielectric constant (â¼40) were formed at Pt compositions > 63 at.%. The Ru-Pt (40-50 at.%) layer also attained an increase in work function of â¼0.3-0.4 eV, leading to an improvement in the leakage currents of the TiO2/Ru-Pt capacitor. These findings suggested that a Ru-Pt layer could serve as a promising electrode for next-generation DRAM capacitors.
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Melanin is a pigment produced from tyrosine in melanocytes. Although melanin has a protective role against UVB radiation-induced damage, it is also associated with the development of melanoma and darker skin tone. Tyrosinase is a key enzyme in melanin synthesis, which regulates the rate-limiting step during conversion of tyrosine into DOPA and dopaquinone. To develop effective RNA interference therapeutics, we designed a melanin siRNA pool by applying multiple prediction programs to reduce human tyrosinase levels. First, 272 siRNAs passed the target accessibility evaluation using the RNAxs program. Then we selected 34 siRNA sequences with ΔG ≥-34.6 kcal/mol, i-Score value ≥65, and siRNA scales score ≤30. siRNAs were designed as 19-bp RNA duplexes with an asymmetric 3' overhang at the 3' end of the antisense strand. We tested if these siRNAs effectively reduced tyrosinase gene expression using qRT-PCR and found that 17 siRNA sequences were more effective than commercially available siRNA. Three siRNAs further tested showed an effective visual color change in MNT-1 human cells without cytotoxic effects, indicating these sequences are anti-melanogenic. Our study revealed that human tyrosinase siRNAs could be efficiently designed using multiple prediction algorithms.
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Accuracy of the Harman measurement largely depends on the heat transfer between the sample and its surroundings, so-called parasitic thermal effects (PTEs). Similar to the material evaluations, measuring thermoelectric modules (TEMs) is also affected by the PTEs especially when measuring under atmospheric condition. Here, we study the correction methods for the Harman measurements with systematically varied samples (both bulk materials and TEMs) at various conditions. Among several PTEs, the heat transfer via electric wires is critical. Thus, we estimate the thermal conductance of the electric wires, and correct the measured properties for a certain sample shape and measuring temperature. The PTEs are responsible for the underestimation of the TEM properties especially under atmospheric conditions (10-35%). This study will be useful to accurately characterize the thermoelectric properties of materials and modules.
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Output power of thermoelectric generators depends on device engineering minimizing heat loss as well as inherent material properties. However, the device engineering has been largely neglected due to the limited flat or angular shape of devices. Considering that the surface of most heat sources where these planar devices are attached is curved, a considerable amount of heat loss is inevitable. To address this issue, here, we present the shape-engineerable thermoelectric painting, geometrically compatible to surfaces of any shape. We prepared Bi2Te3-based inorganic paints using the molecular Sb2Te3 chalcogenidometalate as a sintering aid for thermoelectric particles, with ZT values of 0.67 for n-type and 1.21 for p-type painted materials that compete the bulk values. Devices directly brush-painted onto curved surfaces produced the high output power of 4.0 mW cm-2. This approach paves the way to designing materials and devices that can be easily transferred to other applications.
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Interaction between electrons has long been a focused topic in condensed-matter physics since it has led to the discoveries of astonishing phenomena, for example, high-Tc superconductivity and colossal magnetoresistance (CMR) in strongly-correlated materials. In the study of strongly-correlated perovskite oxides, Nb-doped SrTiO3 (Nb:SrTiO3) has been a workhorse not only as a conducting substrate, but also as a host possessing high carrier mobility. In this work, we report the observations of large linear magnetoresistance (LMR) and the metal-to-insulator transition (MIT) induced by magnetic field in heavily-doped Nb:STO (SrNb0.2Ti0.8O3) epitaxial thin films. These phenomena are associated with the interplay between the large classical MR due to high carrier mobility and the electronic localization effect due to strong spin-orbit coupling, implying that heavily Nb-doped Sr(Nb0.2Ti0.8)O3 is promising for the application in spintronic devices.
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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.
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Vertically ordered hematite nanotubes are considered to be promising photoactive materials for high-performance water-splitting photoanodes. However, the synthesis of hematite nanotubes directly on conducting substrates such as fluorine-doped tin oxide (FTO)/glass is difficult to be achieved because of the poor adhesion between hematite nanotubes and FTO/glass. Here, we report the synthesis of hematite nanotubes directly on FTO/glass substrate and high-performance photoelectrochemical properties of the nanotubes with NiFe cocatalysts. The hematite nanotubes are synthesized by a simple electrochemical anodization method. The adhesion of the hematite nanotubes to the FTO/glass substrate is drastically improved by dipping them in nonpolar cyclohexane prior to postannealing. Bare hematite nanotubes show a photocurrent density of 1.3 mA/cm(2) at 1.23 V vs a reversible hydrogen electrode, while hematite nanotubes with electrodeposited NiFe cocatalysts exhibit 2.1 mA/cm(2) at 1.23 V which is the highest photocurrent density reported for hematite nanotubes-based photoanodes for solar water splitting. Our work provides an efficient platform to obtain high-performance water-splitting photoanodes utilizing earth-abundant hematite and noble-metal-free cocatalysts.
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Detection of gas-phase chemicals finds a wide variety of applications, including food and beverages, fragrances, environmental monitoring, chemical and biochemical processing, medical diagnostics, and transportation. One approach for these tasks is to use arrays of highly sensitive and selective sensors as an electronic nose. Here, we present a high performance chemiresistive electronic nose (CEN) based on an array of metal oxide thin films, metal-catalyzed thin films, and nanostructured thin films. The gas sensing properties of the CEN show enhanced sensitive detection of H2S, NH3, and NO in an 80% relative humidity (RH) atmosphere similar to the composition of exhaled breath. The detection limits of the sensor elements we fabricated are in the following ranges: 534 ppt to 2.87 ppb for H2S, 4.45 to 42.29 ppb for NH3, and 206 ppt to 2.06 ppb for NO. The enhanced sensitivity is attributed to the spillover effect by Au nanoparticles and the high porosity of villi-like nanostructures, providing a large surface-to-volume ratio. The remarkable selectivity based on the collection of sensor responses manifests itself in the principal component analysis (PCA). The excellent sensing performance indicates that the CEN can detect the biomarkers of H2S, NH3, and NO in exhaled breath and even distinguish them clearly in the PCA. Our results show high potential of the CEN as an inexpensive and noninvasive diagnostic tool for halitosis, kidney disorder, and asthma.
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Nariz Electrónica , Biomarcadores , Pruebas Respiratorias , Nanoestructuras , ÓxidosRESUMEN
The wafer-scale synthesis of MoS2 layers with precise thickness controllability and excellent uniformity is essential for their application in the nanoelectronics industry. Here, we demonstrate the atomic layer deposition (ALD) of MoS2 films with Mo(CO)6 and H2S as the Mo and S precursors, respectively. A self-limiting growth behavior is observed in the narrow ALD window of 155-175 °C. Long H2S feeding times are necessary to reduce the impurity contents in the films. The as-grown MoS2 films are amorphous due to the low growth temperature. Post-annealing at high temperatures under a H2S atmosphere efficiently improves the film properties including the crystallinity and chemical composition. An extremely uniform film growth is achieved even on a 4 inch SiO2/Si wafer. These results demonstrate that the current ALD process is well suited for the synthesis of MoS2 layers for application in industry.