181 research outputs found
Intrinsic effects of substitution and intercalation on thermal transport in two-dimensional TiS single crystals
The promising thermoelectric material TiS can be easily chemically doped
and intercalated. We present here studies of single crystals that are
intercalated with excess Ti or Co, or substituted with Ta. We demonstrate the
intrinsic impact of these dopants on the thermal transport in the absence of
grain boundary scattering. We show that Ta doping has the greatest impact on
the thermal scattering rate per ion added, leading to a five-fold reduction in
the lattice thermal conductivity as compared to stoichiometric single crystals.Comment: 5 pages, 2 figure
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A copper-containing oxytelluride as a promising thermoelectric material for waste heat recovery
The new thermoelectric material BiOCuTe exhibits an electrical conductivity of 224 S cm-1 and a Seebeck coefficient of +186 μV K-1 at 373 K, together with an extremely low lattice thermal conductivity of ∼ 0.5 W m-1 K-1. This results in a ZT of 0.42 at 373 K, which increases to 0.66 at the maximum temperature investigated, 673 K
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Ordered-defect sulfides as thermoelectric materials
The thermoelectric behaviour of the transition-metal disulphides n-type NiCr2S4 and p-type CuCrS2 is investigated. Materials prepared by high-temperature reaction were consolidated using cold-pressing and sintering, hot-pressing (HP) in graphite dies or spark-plasma sintering (SPS) in tungsten carbide dies. The consolidation conditions have a marked influence on the electrical transport properties. In addition to the effect on sample density, altering the consolidation conditions results in changes to the sample composition, including the formation of impurity phases. Maximum room-temperature power factors are 0.18 mW m-1 K-2 and 0.09 mW m-1 K-2 for NiCr2S4 and CuCrS2, respectively. Thermal conductivities of ca. 1.4 and 1.2 W m-1 K-1 lead to figures of merit of 0.024 and 0.023 for NiCr2S4 and CuCrS2, respectively
Mg substitution in CuCrO2 delafossite compounds
A detailed investigation of the series CuCr(1-x)MgxO2 (x = 0.0 - 0.05) has
been performed by making high-temperature resistivity and thermopower
measurements, and by performing a theoretical analysis of the latter.
Microstructure characterization has been carried out as well. Upon Mg2+ for
Cr3+ substitution, a concomitant decrease in the electrical resistivity and
thermopower values is found, up to x ~ 0.02 - 0.03, indicating a low solubility
limit of Mg in the structure. This result is corroborated by scanning electron
microscopy observations, showing the presence of MgCr2O4 spinels as soon as x =
0.005. The thermopower is discussed in the temperature-independent correlation
functions ratio approximation as based on the Kubo formalism, and the
dependence of the effective charge carrier density on the nominal Mg
substitution rate is addressed. This leads to a solubility limit of 1.1% Mg in
the delafossite, confirmed by energy dispersive X-ray spectroscopy analysis.Comment: 6 pages, 5 figure
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Amorphous-Like Ultralow Thermal Transport in Crystalline Argyrodite Cu7PS6
Due to their amorphous-like ultralow lattice thermal conductivity both below and above the superionic phase transition, crystalline Cu- and Ag-based superionic argyrodites have garnered widespread attention as promising thermoelectric materials. However, despite their intriguing properties, quantifying their lattice thermal conductivities and a comprehensive understanding of the microscopic dynamics that drive these extraordinary properties are still lacking. Here, an integrated experimental and theoretical approach is adopted to reveal the presence of Cu-dominated low-energy optical phonons in the Cu-based argyrodite Cu7PS6. These phonons yield strong acoustic-optical phonon scattering through avoided crossing, enabling ultralow lattice thermal conductivity. The Unified Theory of thermal transport is employed to analyze heat conduction and successfully reproduce the experimental amorphous-like ultralow lattice thermal conductivities, ranging from 0.43 to 0.58 W m−1 K−1, in the temperature range of 100–400 K. The study reveals that the amorphous-like ultralow thermal conductivity of Cu7PS6 stems from a significantly dominant wave-like conduction mechanism. Moreover, the simulations elucidate the wave-like thermal transport mainly results from the contribution of Cu-associated low-energy overlapping optical phonons. This study highlights the crucial role of low-energy and overlapping optical modes in facilitating amorphous-like ultralow thermal transport, providing a thorough understanding of the underlying complex dynamics of argyrodites
The influence of mobile copper ions on the glass-like thermal conductivity of copper-rich tetrahedrites
Tetrahedrites are promising p-type thermoelectric materials for energy recovery. We present here the first investigation of the structure and thermoelectric properties of copper-rich tetrahedrites, Cu12+xSb4S13 (0 0 consist of two tetrahedrite phases. In-situ neutron diffraction data demonstrate that on heating, the two tetrahedrite phases coalesce into a single tetrahedrite phase at temperatures between 493 and 553 K, and that this transition shows marked hysteresis on cooling. Our structural data indicate that copper ions become mobile above 393 K. Marked changes in the temperature dependence of the electrical and thermal transport properties of the copper-rich phases occur at the onset of copper mobility. Excess copper leads to a significant reduction in the total thermal conductivity, which for the nominal composition Cu14Sb4S13 reaches a value as low as 0.44 W m-1K-1 at room temperature, and to thermoelectric properties consistent with phonon liquid electron crystal (PLEC) behaviour
Tuning the thermoelectric properties of A-site deficient SrTiO3 ceramics by vacancies and carrier concentration
Ceramics based on Sr0.8La0.067Ti0.8Nb0.2O3-δ have been prepared by the mixed oxide route. The La1/3NbO3 component generates ∼13.4% A-site vacancies; this was fixed for all samples. Powders were sintered under air and reducing conditions at 1450 to 1700 K; products were of high density (>90% theoretical). Processing under reducing conditions led to the formation of a Ti1-xNbxO2-y second phase, core-shell structures and oxygen deficiency. X-ray diffraction (XRD) confirmed a simple cubic structure with space group Pm3[combining macron]m. Transmission electron microscopy revealed a high density of dislocations while analytical scanning transmission electron microscopy at atomic resolution demonstrated a uniform distribution of La, Nb and vacancies in the lattice. X-ray photoemission spectroscopy and thermogravimetry showed the oxygen deficiency (δ value) to be ∼0.08 in reduced samples with enhanced carrier concentrations ∼2 × 1021 cm-3. Both carrier concentration and carrier mobility increased with sintering time, giving a maximum figure of merit (ZT) of 0.25. Selective additional doping by La or Nb, with no additional A site vacancies, led to the creation of additional carriers and reduced electrical resistivity. Together these led to enhanced ZT values of 0.345 at 1000 K. The contributions from oxygen vacancies and charge carriers have been investigated independently
Ba6−3x Nd8+2x Ti18O54 Tungsten Bronze: A New High-Temperature n-Type Oxide Thermoelectric
Semiconducting Ba6−3x Nd8+2x Ti18O54 ceramics (with x = 0.00 to 0.85) were synthesized by the mixed oxide route followed by annealing in a reducing atmosphere; their high-temperature thermoelectric properties have been investigated. In conjunction with the experimental observations, atomistic simulations have been performed to investigate the anisotropic behavior of the lattice thermal conductivity. The ceramics show promising n-type thermoelectric properties with relatively high Seebeck coefficient, moderate electrical conductivity, and temperature-stable, low thermal conductivity; For example, the composition with x = 0.27 (i.e., Ba5.19Nd8.54Ti18O54) exhibited a Seebeck coefficient of S 1000K = 210 µV/K, electrical conductivity of σ 1000K = 60 S/cm, and thermal conductivity of k 1000K = 1.45 W/(m K), leading to a ZT value of 0.16 at 1000 K
Optimisation des propriétés anisotropes d'échantillons massifs supraconducteurs Bi2223 texturés par frittage-forgeage
The high-Tc superconducting (Bi,Pb)2Sr2Ca2Cu3O10+x (Bi2223) oxide has been synthesised by a sol-gel route. The calcination and sintering conditions have been optimized in order to synthesise a nearly pure Bi2223 phase, around 94%. The resulting powder has been sinter-forged under air into highly textured discs by optimising the processing conditions. Bars cut from these discs exhibit reproducible transport critical current densities (Jc) having values around 10000 A/cm2 (0 T, 77 K) which are similar to the maximum ones present in the literature. A new way of synthesis, consisting in texturing pellets composed of the Bi2212 phase and secondary phases, was undertaken. The control of the particles size (⊕<63µm) and of the sinter-forging parameters (845°C/100h) allowed to attain Jc around 12500 A/cm2. Ball milling of the sol-gel powder is crucial for increasing its reactivity and in the same time the ratio of Bi2223 phase after sintering-forging. The great quantity of liquid phase produced during texturation allowed the improvement of texture quality via a better alignment of the grains and thus led to strongly increase the critical current densities (20000 A/cm2). In addition, the stacking of several discs was not only shown to be a possible and fast process, but also to produce a massive ceramic with critical current densities almost identical to that obtained on only one disc. The combined analysis (texture/structure/microstructure) treated via the program MAUD presents a great effectiveness to characterize our samples. Thanks to neutron diffraction, a direct relation between the Bi2223 phase content, the cell parameters, the crystallites size , the density of maximum distribution and the transport critical current density was established.L'oxyde supraconducteur à haute Tc (Bi,Pb)2Sr2Ca2Cu3O10+x (Bi2223) a été synthétisé par voie sol-gel. Les conditions de calcination et de frittage ont été optimisées afin d'obtenir la phase Bi2223 avec une pureté voisine de 94%. Cette poudre a été mise sous forme de céramiques texturées par frittage-forgeage sous air. Le cycle de forgeage a été optimisé de manière à synthétiser des disques hautement texturés et d'une grande pureté. Des barreaux extraits de ces disques ont été caractérisés en transport. Les meilleures densités de courant critique (Jc) obtenues sont de l'ordre de 10000 A/cm2 (0 T, 77 K) et rejoignent les valeurs maximales présentes à ce jour dans la littérature. Une nouvelle voie de synthèse, consistant à texturer des pastilles composées de la phase Bi2212 et de phases secondaires, a été entreprise. Le contrôle de la taille de particules (⊕<63µm) et des paramètres de frittage-forgeage (845°C/100h) a permis d'atteindre des Jc de l'ordre de 12500 A/cm2. Le broyage planétaire de la poudre sol-gel brûlée s'est avéré précieux pour augmenter sa réactivité et dans le même temps le taux de phase Bi2223 à l'issue du frittage-forgeage. La grande quantité de phase liquide produite pendant la texturation a permis d'améliorer la qualité de la texture via un meilleur alignement des grains et ainsi d'accroître fortement les densités de courant critiques (20000 A/cm2). Par ailleurs, l'empilement de plusieurs disques est possible et rapide, et aboutit à une céramique massive avec des densités de courant critique quasiment identiques à celles obtenues sur un seul disque. L'analyse combinée texture/structure/microstructure traitée via le programme MAUD s'est révélée être d'une grande efficacité pour caractériser nos échantillons. Grâce à la diffraction neutronique, une relation directe entre le taux de phase Bi2223, les paramètres de maille, la taille des cristallites, la densité de distribution maximale et la densité de courant critique a été établie
Optimisation des propriétés anisotropes d'échantillons massifs supraconducteurs Bi2223 texturés par frittage-forgeage
The high-Tc superconducting (Bi,Pb)2Sr2Ca2Cu3O10+x (Bi2223) oxide has been synthesised by a sol-gel route. The calcination and sintering conditions have been optimized in order to synthesise a nearly pure Bi2223 phase, around 94%. The resulting powder has been sinter-forged under air into highly textured discs by optimising the processing conditions. Bars cut from these discs exhibit reproducible transport critical current densities (Jc) having values around 10000 A/cm2 (0 T, 77 K) which are similar to the maximum ones present in the literature. A new way of synthesis, consisting in texturing pellets composed of the Bi2212 phase and secondary phases, was undertaken. The control of the particles size (⊕<63µm) and of the sinter-forging parameters (845°C/100h) allowed to attain Jc around 12500 A/cm2. Ball milling of the sol-gel powder is crucial for increasing its reactivity and in the same time the ratio of Bi2223 phase after sintering-forging. The great quantity of liquid phase produced during texturation allowed the improvement of texture quality via a better alignment of the grains and thus led to strongly increase the critical current densities (20000 A/cm2). In addition, the stacking of several discs was not only shown to be a possible and fast process, but also to produce a massive ceramic with critical current densities almost identical to that obtained on only one disc. The combined analysis (texture/structure/microstructure) treated via the program MAUD presents a great effectiveness to characterize our samples. Thanks to neutron diffraction, a direct relation between the Bi2223 phase content, the cell parameters, the crystallites size , the density of maximum distribution and the transport critical current density was established.L'oxyde supraconducteur à haute Tc (Bi,Pb)2Sr2Ca2Cu3O10+x (Bi2223) a été synthétisé par voie sol-gel. Les conditions de calcination et de frittage ont été optimisées afin d'obtenir la phase Bi2223 avec une pureté voisine de 94%. Cette poudre a été mise sous forme de céramiques texturées par frittage-forgeage sous air. Le cycle de forgeage a été optimisé de manière à synthétiser des disques hautement texturés et d'une grande pureté. Des barreaux extraits de ces disques ont été caractérisés en transport. Les meilleures densités de courant critique (Jc) obtenues sont de l'ordre de 10000 A/cm2 (0 T, 77 K) et rejoignent les valeurs maximales présentes à ce jour dans la littérature. Une nouvelle voie de synthèse, consistant à texturer des pastilles composées de la phase Bi2212 et de phases secondaires, a été entreprise. Le contrôle de la taille de particules (⊕<63µm) et des paramètres de frittage-forgeage (845°C/100h) a permis d'atteindre des Jc de l'ordre de 12500 A/cm2. Le broyage planétaire de la poudre sol-gel brûlée s'est avéré précieux pour augmenter sa réactivité et dans le même temps le taux de phase Bi2223 à l'issue du frittage-forgeage. La grande quantité de phase liquide produite pendant la texturation a permis d'améliorer la qualité de la texture via un meilleur alignement des grains et ainsi d'accroître fortement les densités de courant critiques (20000 A/cm2). Par ailleurs, l'empilement de plusieurs disques est possible et rapide, et aboutit à une céramique massive avec des densités de courant critique quasiment identiques à celles obtenues sur un seul disque. L'analyse combinée texture/structure/microstructure traitée via le programme MAUD s'est révélée être d'une grande efficacité pour caractériser nos échantillons. Grâce à la diffraction neutronique, une relation directe entre le taux de phase Bi2223, les paramètres de maille, la taille des cristallites, la densité de distribution maximale et la densité de courant critique a été établie
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