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At least 307 records · Page 17

Thermoelectric conversion via laser-induced voltage in highly textured polycrystalline Na{sub x}CoO{sub 2} ceramic

We have studied and analyzed the laser-induced voltage effect in highly c-axis-oriented polycrystalline Na{sub x}CoO{sub 2}. The textured and layered stacking Na{sub x}CoO{sub 2} (x {approx} 0.7) bulks were prepared by a solid-state reaction process. Under the irradiation on Na{sub 0.67}CoO{sub 2} bulk surface with pulsed laser ({lambda} = 248 nm), the induced voltage signals were observed on the inclined surface with rise time 30 ns-43 ns and peak voltage 200 mV-500 mV; the voltage peak values show a linear dependence of laser energy densities. The crystal grains orientation plays a critical role in voltage peak value whether in film or texture bulk. The transverse voltage signal brings the information of thermoelectric anisotropy. In Na{sub x}CoO{sub 2} band structure, the Fermi surface is different in the ab plane and along the c axis, leading to anisotropy of Seebeck coefficient. Additionally, the artificial structure of the inclined surface for highly textured bulk enables us to obtain a transverse voltage on inclined surface. These results demonstrated the layered textured bulk has potential applications in waste-heat conversion via transverse thermoelectric effect.

36 MATERIALS SCIENCE↗

Uncertainty Analysis of Seebeck Coefficient and Electrical Resistivity Characterization

In order to provide a complete description of a materials thermoelectric power factor, in addition to the measured nominal value, an uncertainty interval is required. The uncertainty may contain sources of measurement error including systematic bias error and precision error of a statistical nature. The work focuses specifically on the popular ZEM-3 (Ulvac Technologies) measurement system, but the methods apply to any measurement system. The analysis accounts for sources of systematic error including sample preparation tolerance, measurement probe placement, thermocouple cold-finger effect, and measurement parameters; in addition to including uncertainty of a statistical nature. Complete uncertainty analysis of a measurement system allows for more reliable comparison of measurement data between laboratories.

Seebeck effect↗

Expression of interfacial Seebeck coefficient through grain boundary engineering with multi-layer graphene nanoplatelets

Energy filtering has been a long-sought strategy to enhance a thermoelectric material's figure of merit zT through improving its power factor. Here we show a composite of multi-layer graphene nanoplatelets (GNP) and n-type Mg 3 Sb 2 leads to the expression of an energy filtering like effect demonstrated by an increase in the material's Seebeck coefficient and maximum power factor, without impact on the material's carrier concentration. We analyse these findings from the perspective of a heterogeneous material consisting of grain and grain boundary phases, instead of a more traditional and common analysis that assumes a homogeneously transporting medium. An important implication of this treatment is that it leads to the development of an interfacial Seebeck coefficient term, which can explain the observed increase in the material's Seebeck coefficient. The contribution of this interfacial Seebeck coefficient to the overall Seebeck coefficient is determined by the relative temperature drop across the grain boundary region compared to that of the bulk material. In Te doped Mg 3 Sb 2 we show the introduction of GNP increases the interfacial thermal resistance of grain boundaries, enhancing the contribution of the interfacial Seebeck coefficient arising from grain boundaries to the overall Seebeck coefficient. Without significant detriment to the electrical conductivity this effect results in a net increase in maximum power factor. This increased interfacial thermal resistance also leads to the synergistic reduction of the total thermal conductivity. As a result, we enhance zT of the Mg 3 Sb 2 to a peak value of 1.7 near 750 K. Considering the two-dimensional nature of the grain boundary interface, this grain boundary engineering strategy could be applied to a few thermoelectric systems utilizing various two-dimensional nanomaterials.

42 ENGINEERING↗

Analysis of Residual Acceleration Effects on Transport and Segregation During Directional Solidification of Tin-Bismuth in the MEPHISTO Furnace Facility

The objective of this work is to approach the problem of determining the transport conditions (and effects of residual acceleration) during the plane-front directional solidification of a tin-bismuth alloy under low gravity conditions. The work involves using a combination of 2- and 3-D numerical models, scaling analyses, ID models and the results of ground-based and low-gravity experiments. The latter are to be conducted during the MEPHISTO experiment scheduled for USMP-3 in early 1996. The models will be used to predict the response of the transport conditions and consequent solute segregation in directionally solidifying tin-bismuth melt. Real-time Seebeck voltage variations across a Sn-Bi melt during directional solidification in MEPHISTO on USMP-1 show a distinct variation which can be correlated with thruster firings. The Seebeck voltage measurement is related to the response of the instantaneous average melt composition at the melt-solid interface. This allows a direct comparison of numerical simulations with the Seebeck signals obtained on USMP-1. The effects of such accelerations on composition for a directionally solidifying Sn-Bi alloy have been simulated numerically. USMP-1 acceleration data was used to assist in our choice of acceleration magnitude and orientation. The results show good agreement with experimental observations. The USMP-3 experiments took place earlier this year (February 22 through March 6). There were several differences between the USMP-3 experiments as compared to USMP-1. Firstly a more concentrated alloy was solidified and, secondly, Primary Reaction Control System thruster burns were requested at particular times during four separate growth runs. This allowed us to monitor the response Seebeck response under well-characterized growth conditions. In addition, we carried out simulations during the experiment in order to interpret the Seebeck signal. Preliminary results are described here.

Alexander J. Iwan D.↗

The influence of non-idealities on the thermoelectric power factor of nanostructured superlattices

Cross-plane superlattices composed of nanoscale layers of alternating potential wells and barriers have attracted great attention for their potential to provide thermoelectric power factor improvements and higher ZT figure of merit. Previous theoretical works have shown that the presence of optimized potential barriers could provide improvements to the Seebeck coefficient through carrier energy filtering, which improves the power factor by up to 40%. However, experimental corroboration of this prediction has been extremely scant. In this work, we employ quantum mechanical electronic transport simulations to outline the detrimental effects of random variation, imperfections, and non-optimal barrier shapes in a superlattice geometry on these predicted power factor improvements. Thus, we aim to assess either the robustness or the fragility of these theoretical gains in the face of the types of variation one would find in real material systems. We show that these power factor improvements are relatively robust against: overly thick barriers, diffusion of barriers into the body of the wells, and random fluctuations in barrier spacing and width. However, notably, we discover that extremely thin barriers and random fluctuation in barrier heights by as little as 10% is sufficient to entirely destroy any power factor benefits of the optimized geometry. Our results could provide performance optimization routes for nanostructured thermoelectrics and elucidate the reasons why significant power factor improvements are not commonly realized in superlattices, despite theoretical predictions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Enhanced power factor of higher manganese silicide via melt spin synthesis method

We report on the thermoelectric properties of the Higher Manganese Silicide MnSi₁.₇₅ (HMS) synthesized by means of a one-step non-equilibrium method. The ultrahigh cooling rate generated from the melt-spin technique is found to be effective in reducing second phases, which are inevitable during the traditional solid state diffusion processes. Aside from being detrimental to thermoelectric properties, second phases skew the revealing of the intrinsic properties of this class of materials, for example the optimal level of carrier concentration. With this melt-spin sample, we are able to formulate a simple model based on a single parabolic band that can well describe the carrier concentration dependence of the Seebeck coefficient and power factor of the data reported in the literature. An optimal carrier concentration around 5x10²⁰ cm⁻³ at 300 K is predicted according to this model. The phase-pure melt-spin sample shows the largest power factor at high temperature, resulting in the highest zT value among the three samples in this paper; the maximum value is superior to those reported in the literatures.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Photo-transport properties of Pb{sub 2}CrO{sub 5} single crystals

We report photo-thermoelectric transport phenomena in Pb{sub 2}CrO{sub 5} single crystals. Without illumination, this material exhibits an insulating behavior characterized by an activation-type temperature variation of the electrical conductivity. The Seebeck coefficient contrastingly shows a crossover from high-temperature insulating to low-temperature metallic behavior, which is attributed to degenerate carriers in a donor level. We have found that under illumination, both the conductivity and the Seebeck coefficient increase in magnitude with increasing photon flux density in the degenerate-conduction regime. This result is difficult to understand within a simple photo-doping effect, which usually leads to a decrease in the Seebeck coefficient under illumination. The observed phenomenon is discussed in terms of a two-carrier contribution to the transport properties.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

High Thermoelectric Performance through Crystal Symmetry Enhancement in Triply Doped Diamondoid Compound Cu 2 SnSe 3

The presence of high crystallographic symmetry and nanoscale defects are favorable for thermoelectrics. With proper electronic structures, a highly symmetric crystal tends to possess multiple carrier channels and promote electrical conductivity without sacrificing Seebeck coefficient. In addition, nanoscale defects can effectively scatter acoustic phonons to suppress thermal conductivity. Here, we report that the triple doping of Cu 2 SnSe 3 leads to a high ZT value of 1.6 at 823 K for Cu 1.85 Ag 0.15 (Sn 0.88 Ga 0.1 Na 0.02 )Se 3 , and a decent average ZT (ZT ave ) value of 0.7 is also achieved for Cu 1.85 Ag 0.15 (Sn 0.93 Mg 0.06 Na 0.01 )Se 3 from 475 to 823 K. Our study reveals: (1) Ag doping on Cu sites generates numerous point defects and greatly decreases lattice thermal conductivity. (2) Doping Mg or Ga converts the monoclinic Cu 2 SnSe 3 into a cubic structure. This symmetry enhancing leads to increase in the effective mass from 0.8 m e to 2.6 m e (m e , free electron mass) and the power factor from 4.3 μW/cm –1 K –2 for Cu 2 SnSe 3 to 11.6 μW/cm –1 K –2 . (3) Na doping creates dense dislocation arrays and nanoprecipitates, which strengthens the phonon scattering. (4) Pair distribution function analysis shows localized symmetry breakdwon in the cubic Cu 1.85 Ag 0.15 (Sn 0.88 Ga 0.1 Na 0.02 )Se 3 . Furthermore, the present work provides a standpoint to design promising thermoelectric materials by synergistically manipulating crystal symmetry and nanoscale defects.

36 MATERIALS SCIENCE↗

Thermoelectric transport properties of diamond-like Cu{sub 1−x}Fe{sub 1+x}S{sub 2} tetrahedral compounds

Polycrystalline samples with the composition of Cu{sub 1−x}Fe{sub 1+x}S{sub 2} (x = 0, 0.01, 0.03, 0.05, 0.1) were synthesized by a melting-annealing-sintering process. X-ray powder diffraction reveals all the samples are phase pure. The backscattered electron image and X-ray map indicate that all elements are distributed homogeneously in the matrix. The measurements of Hall coefficient, electrical conductivity, and Seebeck coefficient show that Fe is an effective n-type dopant in CuFeS{sub 2}. The electron carrier concentration of Cu{sub 1−x}Fe{sub 1+x}S{sub 2} is tuned within a wide range leading to optimized power factors. The lattice phonons are also strongly scattered by the substitution of Fe for Cu, leading to reduced thermal conductivity. We use Debye approximation to model the low temperature lattice thermal conductivity. It is found that the large strain field fluctuation introduced by the disordered Fe ions generates extra strong phonon scatterings for lowered lattice thermal conductivity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Preparation and Thermoelectric Properties of the Skutterudite-Related Phase Ru(0.5)Pd(0.5)Sb3

A new skutterudite phase Ru(0.5)Pd(0.5)Sb3 was prepared. This new phase adds to a large number of already known materials with the skutterudite structure which have shown good potential for thermoelectric applications. Single phase, polycrystalline samples were prepared and characterized by x-ray analysis, electron probe microanalysis, density, sound velocity, thermal-expansion coefficient, and differential thermal analysis measurements. Ru(0.5)Pd(0.5)Sb3 has a cubic lattice, space group Im3 (T(sup 5, sub h)), with a = 9.298 A and decomposes at about 920 K. The Seebeck coefficient, the electrical resistivity, the Hall effect, and the thermal conductivity were measured on hot-pressed samples over a wide range of temperatures. Preliminary results show that Ru(0.5)Pd(0.5)Sb3 behaves as a heavily doped semiconductor with an estimated band gap of about 0.6 eV. The lattice thermal conductivity of Ru(0.5)Pd(0.5)Sb3 is substantially lower than that of the binary isostructural compounds CoSb3 and IrSb3. The unusually low thermal conductivity might be explained by additional hole and charge transfer phonon scattering in this material. The potential of this material for thermoelectric applications is discussed.

Caillat, T.↗

Static Polystyrene Gate Charge Density Modulation of Dinaphthothienothiophene with Tetrafluorotetracyanoquinodimethane Layer Doping: Evidence from Conductivity and Seebeck Coefficient Measurements and Correlations

We relate the static charging of organic field effect transistor (OFET) gate dielectric polymers, the resulting change in threshold voltage shift, and the modulation of thermoelectric properties of the transistor semiconductor. We utilize a bottom gate OFET structure with cross-linkable polystyrene and plain polystyrene (XLPS/PS) bilayer dielectrics and dinaphthothienothiophene (DNTT) organic molecular semiconductor with tetrafluorotetracyanoquinodimethane (F4TCNQ) doping layer. Conductivity and Seebeck coefficient are measured before and after charging. We find that the conductivity increases significantly, while the Seebeck coefficient decreases correspondingly in a trend of S ∝ ln(σ) after the dielectrics were negatively charged, resulting in an average of fivefold increase in power factor at the maximum charging level. Additionally, temperature-dependent conductivity measurements show that the activation energy decreases with the increasing conductivity. We calculate the Seebeck coefficient based on the activation energy and find the result is consistent with the Mott mobility edge model. This work confirms the charging mechanism in our previous published work, including the location of static charges in the bulk of the dielectric, and demonstrates modulation and enhancement of the thermoelectric properties of organic thermoelectric materials by adjacent chargeable dielectrics without changing the molecular microstructure or applying external gate voltage during operation.

static gate, Seebeck coefficient, organic semicond↗

Advances in Atomic Layer Deposition (ALD) Nanolaminate Synthesis of Thermoelectric Films in Porous Templates for Improved Seebeck Coefficient

Thermoelectrics is a green renewable energy technology which can significantly contribute to power generation due to its potential in generating electricity out of waste heat. The main challenge for the development of thermoelectrics is its low conversion efficiency. One key strategy to improve conversion efficiency is reducing the thermal conductivity of thermoelectric materials. In this paper, the state-of-the-art progresses made in improving thermoelectric materials are reviewed and discussed, focusing on phononic engineering via applying porous templates and ALD deposited nanolaminates structure. The effect of nanolaminates structure and porous templates on Seebeck coefficient, electrical conductivity and thermal conductivity, and hence in figure of merit zT of different types of materials system, including PnCs, lead chalcogenide-based nanostructured films on planar and porous templates, ZnO-based superlattice, and hybrid organic-inorganic superlattices, will be reviewed and discussed.

36 MATERIALS SCIENCE↗

High Thermoelectric Performance in Supersaturated Solid Solutions and Nanostructured n-Type PbTe-GeTe

Sb-doped and GeTe-alloyed n-type thermoelectric materials that show an excellent figure of merit ZT in the intermediate temperature range (400–800 K) are reported. The synergistic effect of favorable changes to the band structure resulting in high Seebeck coefficient and enhanced phonon scattering by point defects and nanoscale precipitates resulting in reduction of thermal conductivity are demonstrated. The samples can be tuned as single-phase solid solution (SS) or two-phase system with nanoscale precipitates (Nano) based on the annealing processes. The GeTe alloying results in band structure modification by widening the bandgap and increasing the density-ofstates effective mass of PbTe, resulting in significantly enhanced Seebeck coefficients. The nanoscale precipitates can improve the power factor in the low temperature range and further reduce the lattice thermal conductivity (κ lat ). Specifically, the Seebeck coefficient of Pb 0.988 Sb 0.012 Te–13%GeTe–Nano approaches -280 μV K -1 at 673 K with a low κ lat of 0.56 W m -1 K -1 at 573 K. Consequently, a peak ZT value of 1.38 is achieved at 623 K. Furthermore, a high average ZT avg value of ≈1.04 is obtained in the temperature range from 300 to 773 K for n-type Pb 0.988 Sb 0.012 Te–13%GeTe–Nano.

36 MATERIALS SCIENCE↗

The Shubnikov-de Haas effect and thermoelectric properties of Tl-doped Sb{sub 2}Te{sub 3} and Bi{sub 2}Se{sub 3}

The influence of doping with Tl on the Shubnikov-de Haas effect at T = 4.2 K in magnetic fields up to 38 T in p-Sb{sub 2−x}Tl{sub x}Te{sub 3} (x = 0, 0.005, 0.015, and 0.05) and n-Bi{sub 2−x}Tl{sub x}Se{sub 3} (x = 0, 0.01, 0.02, 0.04, and 0.06) single crystals is investigated. Extreme cross-sections of the Fermi surface in both materials decrease upon doping with Tl: the hole concentration decreases in Sb{sub 2−x}Tl{sub x}Te{sub 3} due to the donor effect of Tl and the electron concentration in n-Bi{sub 2−x}Tl{sub x}Se{sub 3} decreases due to the acceptor effect of Tl. The temperature dependences of the Seebeck coefficient, electrical conductivity, thermal conductivity, and dimensionless thermoelectric figure of merit in a temperature range of 77–300 K are measured. The thermal conductivity and electrical conductivity decrease upon doping with Tl both in p-Sb{sub 2−x}Tl{sub x}Te{sub 3} and in n-Bi{sub 2−x}Tl{sub x}Se{sub 3}. The Seebeck coefficient increases in all compositions upon an increase in doping over the entire measured temperature range. The thermoelectric figure of merit increases upon doping with Tl.

36 MATERIALS SCIENCE↗

Thermoelectric properties of lanthanum sulfide

The Seebeck coefficient, electrical resistivity, thermal conductivity, and Hall effect have been studied in gamma-phase La(3-x)S4(LaS/y/) for compositions with x in the range from 0.04 to 0.3 (y in the range from 1.35 to 1.48) in order to ascertain its suitability for high-temperature (300 to 1400 K) thermoelectric energy conversion. In this temperature and composition range the material behaves as an extrinsic semiconductor whose degenerate carrier concentration is controlled by the stoichiometric ratio of La to S. A maximum figure-of-merit (Z) of approximately 0.0005 per K at a composition x = 0.3, y = 1.48 (LaS/1.48/) was obtained.

Wood, C.↗

Thermoelectric Properties of Lanthanum Sulfide

Report describes measurement of Seebeck coefficient, electrical resistivity, thermal conductivity, and Hall effect in gamma-phase lanthanum sulfide with composition of La3-x S4. Results of study, part of search for high-temperature thermoelectric energy-conversion materials, indicate this sulfide behaves like extrinsic semiconductor over temperature range of 300 to 1,400 K, with degenerate carrier concentration controlled by stoichiometric ratio of La to S.

Wood, C.↗

Properties of Single Crystalline Semiconducting CoSb3

A study of the thermoelectric properties of the skutterudite compound CoSb3 was carried out on single crystals grown by the Bridgman gradient freeze technique. p- and n-type samples were obtained over a wide range of carrier concentration. Undoped As-grown crystals show p-type conductivity while n-type samples were obtained by addition of Te or Pd. Samples were characterized by x-ray diffractometry, electron microprobe analysis, and density measurements. The physical properties of CoSb3 such as linear thermal expansion coefficient, sound velocity, and Debye temperature were also determined and are presented. Seebeck coefficient, electrical resistivity, thermal conductivity, and Hall effect measurements were performed between room temperature and about 900 K. Exceptionally high Hall mobilities were obtained on p-type samples with a maximum room-temperature Hall mobility of 3300 sq cm/V.s at a carrier concentration of 1 x 10(exp 17)/cc. The results of the transport property measurements are discussed and are in agreement with some recent predictions based on band structure calculations. The potential of CoSb3 for thermoelectric applications is evaluated.

Caillat, T.↗

Thermoelectric properties of n-type polycrystalline BixSb2-xTe3 alloys

(BixSbl-x)2Te3(.5 = x = .7) polycrystalline samples were synthesized using a combination of melting and powder metallurgy techniques. The samples were hot pressed in graphite dies and cut perpendicular and parallel to the pressing direction. Samples were examined by microprobe analysis to determine their atomic composition. The thermoelectric properties were measured at room temperature in both directions. These properties include Seebeck coefficient, thermal conductivity, electrical resistivity, and Hall effect. The thermoelectric figure-of-merit, ZT, was calculated fiom these properties.

thermoelectric power generation segmented↗