ABSTRACT
Many monumental breakthroughs in p-type PbTe thermoelectrics are driven by optimizing a Pb0.98Na0.02Te matrix. However, recent works found that x > 0.02 in Pb1-xNaxTe further improves the thermoelectric figure of merit, zT, despite being above the expected Na solubility limit. We explain the origins of improved performance from excess Na doping through computation and experiments on Pb1-xNaxTe with 0.01 ≤ x ≤ 0.04. High temperature X-ray diffraction and Hall carrier concentration measurements show enhanced Na solubility at high temperatures when x > 0.02 but no improvement in carrier concentration, indicating that Na is entering the lattice but is electrically compensated by high intrinsic defect concentrations. The higher Na concentration leads to band convergence between the light L and heavy Σ valence bands in PbTe, suppressing bipolar conduction and increasing the Seebeck coefficient. This results in a high temperature zT nearing 2 for Pb0.96Na0.04Te, â¼25% higher than traditionally reported values for pristine PbTe-Na. Further, we apply a phase diagram approach to explain the origins of increased solubility from excess Na doping and offer strategies for repeatable synthesis of high zT Na-doped materials. A starting matrix of simple, high performing Pb0.96Na0.04Te synthesized following our guidelines may be superior to Pb0.98Na0.02Te for continued zT optimization in p-type PbTe materials.
ABSTRACT
The misfit monolayered sulfides, (GdS)1.20NbS2, (DyS)1.22NbS2, (Gd0.1Dy0.9S)1.21NbS2, (Gd0.2Dy0.8S)1.21NbS2, and (Gd0.5Dy0.5S)1.21NbS2 and the misfit bilayered sulfide (GdS)0.60NbS2 were synthesized via sulfurization under flowing CS2/H2S gas and consolidated by pressure-assisted sintering. The thermoelectric properties of the monolayered and bilayered sulfides perpendicular (in-plane) and parallel (out-of-plane) to the pressing direction were investigated over a temperature range of 300-873 K. The crystal grains in all the sintered samples were preferentially oriented perpendicular to the pressing direction, which resulted in highly anisotropic electrical and thermal transport properties. All the sintered samples exhibited degenerate n-type semiconductor-like behavior, leading to a large thermoelectric power factor. The misfit layered structure yielded low lattice thermal conductivity. The evolution of the monolayered structures into bilayered structures affected their thermoelectric properties. The thermoelectric figure of merit (ZT) of monolayered (GdS)1.20NbS2 was higher than that of bilayered (GdS)0.60NbS2 due to the larger power factor and lower lattice thermal conductivity of (GdS)1.20NbS2. The lattice thermal conductivity of the monolayered sulfide was lower in (Gd x Dy1-x S)1.2+q NbS2 solid solutions. The large power factor and low lattice thermal conductivity allowed a ZT value of 0.13 at 873 K in (Gd0.5Dy0.5S)1.21NbS2 perpendicular to the pressing direction.
ABSTRACT
Sulfides are promising candidates for environment-friendly and cost-effective thermoelectric materials. In this article, we review the recent progress in all-length-scale hierarchical architecturing for sulfides and chalcogenides, highlighting the key strategies used to enhance their thermoelectric performance. We primarily focus on TiS2-based layered sulfides, misfit layered sulfides, homologous chalcogenides, accordion-like layered Sn chalcogenides, and thermoelectric minerals. CS2 sulfurization is an appropriate method for preparing sulfide thermoelectric materials. At the atomic scale, the intercalation of guest atoms/layers into host crystal layers, crystal-structural evolution enabled by the homologous series, and low-energy atomic vibration effectively scatter phonons, resulting in a reduced lattice thermal conductivity. At the nanoscale, stacking faults further reduce the lattice thermal conductivity. At the microscale, the highly oriented microtexture allows high carrier mobility in the in-plane direction, leading to a high thermoelectric power factor.
ABSTRACT
The authors wish to make the following corrections to this paper [1]. [...].
ABSTRACT
Porous titanium dioxide synthesized with a bicontinuous surfactant template is a promising method that leads to a high active surface area electrode. The template used is based on a water/isooctane/dioctyl sodium sulfosuccinate salt together with lecithin. Several parameters were varied during the synthesis to understand and optimize channel formation mechanisms. The material is patterned in stacked conical channels, widening towards the centre of the grains. The active surface area increased by 116 % when the concentration of alkoxide precursors was decreased and increased by 241 % when the template formation temperature was decreased to 10 °C. Increasing the oil phase viscosity tends to widen the pore aperture, thus decreasing the overall active surface area. Changing the phase proportions alters the microemulsion integrity and disrupts channel formation.
ABSTRACT
ZnO is a promising high figure-of-merit (ZT) thermoelectric material for power harvesting from heat due to its high melting point, high electrical conductivity σ, and Seebeck coefficient α, but its practical use is limited by a high lattice thermal conductivity κ(L). Here, we report Al-containing ZnO nanocomposites with up to a factor of 20 lower κ(L) than non-nanostructured ZnO, while retaining bulklike α and σ. We show that enhanced phonon scattering promoted by Al-induced grain refinement and ZnAl(2)O(4) nanoprecipitates presages ultralow κ â¼ 2 Wm( -1) K(-1) at 1000 K. The high αâ¼ -300 µV K(-1) and high σ â¼ 1-10(4) Ω(-1 )m(-1) result from an offsetting of the nanostructuring-induced mobility decrease by high, and nondegenerate, carrier concentrations obtained via excitation from shallow Al donor states. The resultant ZT â¼ 0.44 at 1000 K is 50% higher than that for the best non-nanostructured counterpart material at the same temperature and holds promise for engineering advanced oxide-based high-ZT thermoelectrics for applications.
