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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

A robust high sensitivity scanning thermal probe for simultaneous microscale thermal and thermoelectric property mapping

Scanning Thermal Microscopy (SThM) provides efficient thermal property measurement with micro- or nanoscale spatial resolution. However, the sensitivity and accuracy of state-of-the-art thermal probes have been limited by excessive thermal contact resistance between the probe and sample. Introduced herein is a robust thermal microprobe that can increase the probe-sample contact force by more than two orders of magnitude, thereby reducing the probe-sample thermal contact resistance by as much as 96% and increasing measurement sensitivity by more than 240% compared to a commercial thermal probe with the same dimensions and measurement principle. The relationship between the probe-sample thermal contact resistance, thermal exchange radius, and sample thermal conductivity is determined experimentally. Simultaneous measurement of thermal conductivity and Seebeck coefficient with unprecedented sensitivity is demonstrated using the enhanced scanning thermal microprobe on samples of an extended range of thermal conductivity up to 18 W/m K, increasing the range of samples applicable to SThM when compared to the conventional commercial probe with diminished measurement sensitivity above ~10 W/m K. The probe is further demonstrated by simultaneously mapping thermal conductivity and Seebeck coefficient as a function of depth from the irradiated surface of an ion-irradiated bulk nanostructured thermoelectric material. In addition to enabling microscale thermal conductivity and Seebeck coefficient measurement of materials previously not applicable to SThM, the probe can also facilitate high-throughput characterization of combinatorial materials to aid the rapid discovery of compositions and processing conditions that yield highly desired thermal and thermoelectric properties.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Ultralow Thermal Conductivity, Multiband Electronic Structure and High Thermoelectric Figure of Merit in TlCuSe

The entanglement of lattice thermal conductivity, electrical conductivity, and Seebeck coefficient complicates the process of optimizing thermoelectric performance in most thermoelectric materials. Semiconductors with ultralow lattice thermal conductivities and high power factors at the same time are scarce but fundamentally interesting and practically important for energy conversion. In this work, an intrinsic p-type semiconductor TlCuSe that has an intrinsically ultralow thermal conductivity (0.25 W m -1 K -1 ), a high power factor (11.6 μ W cm -1 K -2 ), and a high figure of merit, ZT (1.9) at 643 K is described. The weak chemical bonds, originating from the filled antibonding orbitals p-d* within the edge-sharing CuSe 4 tetrahedra and long Tl-Se bonds in the PbClF-type structure, in conjunction with the large atomic mass of Tl lead to an ultralow sound velocity. Strong anharmonicity, coming from Tl + lone-pair electrons, boosts phonon-phonon scattering rates and further suppresses lattice thermal conductivity. The multiband character of the valence band structure contributing to power factor enhancement benefits from the lone-pair electrons of Tl + as well, which modify the orbital character of the valence bands, and pushes the valence band maximum off the Gamma-point, increasing the band degeneracy. The results provide new insight on the rational design of thermoelectric materials.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Hierarchical microstructure of Yb-filled skutterudites through ultrasonically atomized spherical powders for enhanced thermoelectric performance

Hierarchical microstructures are widely explored as a strategy to reduce lattice thermal conductivity in thermoelectric materials while preserving favorable electronic transport. Here we demonstrate that ultrasonic atomization of precursor powders provides an intrinsic pathway to generate such architectures in n-type Yb0.3Co4Sb12 skutterudites. Materials were synthesized by both conventional sealed-ampoule and ultrasonic atomization routes, each yielding essentially single-phase skutterudite after densification. However, the atomized spherical powders undergo a distinct reaction-driven microstructural evolution during thermal treatment prior to densification. Electron microscopy reveals that the skutterudite phase within the particles induces swelling, cracking, and fragmentation of the droplets before consolidation. Multimodal structural and microstructural characterizations show that densification of these fragmented powders produces a hierarchical microstructure consisting of submicron grains, micrometer-scale faceted crystallites, and powder-derived domains separated by oxide-decorated boundaries. Comprehensive thermoelectric transport measurements evidence that this multiscale architecture lowers the lattice thermal conductivity while maintaining favorable electronic transport, leading to an average ~10% enhancement in the thermoelectric figure of merit. Complementary 121Sb Mössbauer spectroscopy further indicates lattice softening in the atomized material. These results demonstrate that ultrasonic atomization provides an effective route to engineer hierarchical microstructures in skutterudite thermoelectrics and offers a promising strategy for tailoring thermal transport in energy-conversion materials.

Bouteiller, Hugo [ORNL] (ORCID:0009000421322962)↗
DOE OSTI2020

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↗
DOE OSTI2023

Effect of Sn oxides on the thermal conductivity of polycrystalline SnSe

SnSe is a promising thermoelectric material, with intrinsically low lattice thermal conductivity, κL. Surprisingly, in several reports, polycrystalline samples are found to have a higher thermal conductivity than single crystals. This disparity has been attributed to trace amounts of thermally conductive Sn oxides at the grain boundaries of polycrystalline samples. The same culprit was recently proposed to explain the reduction of κL in purified, oxide-free, SnSe polycrystals. Here, we test this hypothesis by: (i) tuning the type of oxide in SnSe by exploiting thermodynamic stability regions, since Sn-rich or Sn-poor compositions favour the formation of SnO or SnO 2 , respectively; and (ii) varying the quantity of SnO 2 by intentionally oxidizing SnSe powder before consolidation, to obtain samples with quantifiable amounts - up to 15% - of SnO 2 . We find that the κL of SnSe is impervious to changes in the type or the amount of Sn oxide present in the samples. Our results show that a simple “rule of mixtures” cannot be used to estimate the effect of grain boundary oxides on the thermal conductivity of SnSe. These results call for an improved understanding of the intriguing thermal transport mechanisms in SnSe and numerous other systems where a two-phase transport is presumed.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Chemistry, Structure, and Function of Lone Pairs in Extended Solids

The lone pair has been a known feature of the electronic structure of molecules for over 100 years. Beginning with the pioneering work of Lewis and others that was later developed into useful guidelines for predicting molecular structure, lone pairs and their steric consequences are now taught at the very earliest stages of a chemistry education. In the crystalline solid state, lone pairs have perhaps had a less visible yet equally consequential role, with a significant impact on a range of properties and functionalities. Important properties associated with s 2 electron-derived lone pairs include their role in creating conditions favorable for ion transport, in the formation and correlation of local dipoles and the resulting polar behavior leading to ferroics and multiferroics, in increasing the refractive index of glass, in reducing the thermal conductivity of thermoelectric materials, and in breaking local symmetry permitting second-harmonic light generation.. In recent years, the role of the lone pair in developing the electronic structure of some topological quantum materials has also been recognized. While structural distortions due to lone pairs have traditionally been characterized through their crystallography, recent advances in scattering and spectroscopy have revealed the presence of local lone pair-driven distortions that do not correlate over long length scales. The role of these crystallographically “hidden” lone pairs, their detection, and their impact on properties have become a growing body of work in the literature. Hidden lone pairs are an effective argument for considering a role for lone pairs that goes beyond their being objects that occupy space in the coordination polyhedra of cations. This Account introduces the chemistry of lone pairs in extended crystalline solids, including a discussion of when they are stereochemically active, how they manifest in the structure, and how their chemistry can be tuned by the chemical environment around them. Eventually, all of these factors work in unison to help develop and tune properties of interest. Certain specific examples of structure–property relationships in materials that are driven by lone pair behavior are described here, including the potential impact of lone pairs on the optical and electronic properties of hybrid halide perovskite compounds that are relevant to their photovoltaic applications. Here, we highlight the role of lone pairs in the dielectric behavior of geometrically frustrated pyrochlores, the temperature-dependent optoelectronic behavior of halide perovskites, the polar phase transitions in lead-free ferroelectric perovskites, and the compositional insulator-to-metal transition in ruthenium pyrochlores. The theme underpinning this Account is that the lone pair can be considered to be a powerful design element for a broad range of material function.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Size- and Temperature-Dependent Suppression of Phonon Thermal Conductivity in Carbon Nanotube Thermoelectric Films

Heat transport in nanoscale carbon materials such as carbon nanotubes and graphene is normally dominated by phonons. Here, measurements of in-plane thermal conductivity, electrical conductivity, and thermopower are presented from 77–350 K on two films with thickness <100 nm formed from semiconducting single-walled carbon nanotubes. These measurements are made with silicon–nitride membrane thermal isolation platforms. The two films, formed from disordered networks of tubes with differing tube and bundle size, have very different thermal conductivity. One film matches a simple model of heat conduction assuming constant phonon velocity and mean free path, and 3D Debye heat capacity with a Debye temperature of 770 K. The second film shows a more complicated temperature dependence, with a dramatic drop in a relatively narrow window near 200 K where phonon contributions to thermal conductivity essentially vanish. This causes a corresponding large increase in thermoelectric figure-of-merit at the same temperature. A better understanding of this behavior can allow significant improvement in thermoelectric efficiency of these low-cost earth-abundant, organic electronic materials. Finally, heat and charge conductivity near room temperature is also presented as a function of doping, which provides further information on the interaction of dopant molecules and phonon transport in disordered nanotube films.

36 MATERIALS SCIENCE↗
DOE OSTI2020

All-Inorganic Halide Perovskites as Potential Thermoelectric Materials: Dynamic Cation off-Centering Induces Ultralow Thermal Conductivity

Halide perovskites are anticipated to impact next generation high performance solar cells because of their extraordinary charge transport and optoelectronic properties. However, their thermal transport behavior has received limited attention. In this work, we studied the thermal transport and thermoelectric properties of the CsSnBr 3–x I x perovskites. We find a strong correlation between lattice dynamics and an ultralow thermal conductivity for series CsSnBr 3–x I x reaching 0.32 Wm –1 K –1 at 550 K. The CsSnBr 3–x I x also possess a decent Seebeck coefficient and controllable electrical transport properties. The crystallography data and theoretical calculations suggest the Cs atom deviates from its ideal cuboctahedral geometry imposed by the perovskite cage and behaves as a heavy atom rattling oscillator. This off-center tendency of Cs, together with the distortion of SnX 6 (X = Br or I) octahedra, produces a highly dynamic and disordered structure in CsSnBr 3–x I x , which gives rise to a very low Debye temperature and phonon velocity. Moreover, the low temperature heat capacity data suggests strong coupling between the low frequency optical phonons and heat carrying acoustical phonons. In conclusion, this induces strong phonon resonance scattering that induces the ultralow lattice thermal conductivity of CsSnBr 3–x I x .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Understanding the thermally activated charge transport in NaPb m SbQ m+2 (Q = S, Se, Te) thermoelectrics: weak dielectric screening leads to grain boundary dominated charge carrier scattering

Many thermoelectric materials feature irregular electrical conductivity with thermally activated transport below ~600 K and metallic behavior at high temperatures, despite possessing degenerate carrier concentrations. The suppression of the electrical conductivity ultimately degrades the thermoelectric performance on the cold side and limits the device energy conversion efficiency. As such, establishing the origin of the low temperature scattering and developing strategies to mitigate its effect are paramount issues. To date, the correct microscopic description of the low temperature carrier scattering remains an open issue, and there is little work addressing why some thermoelectric materials are more susceptible to the deleterious behavior. Here, we use the promising thermoelectric alloys of PbQ and NaSbQ 2 (Q = S, Se, Te) as model systems to address these concerns. We directly show the thermally activated transport stems from the scattering of charge carriers by the grain boundaries (GBs), and that the expected metallic electrical conductivity is recovered by preparing large grained samples with reduced densities of GBs. We furthermore study the electrical properties NaPb m SbSe m+2 as a function of NaSbSe 2 fraction, as well as those of the chalcogenide analogues, PbTe–NaSbTe 2 and PbS–NaSbS 2 , and demonstrate that the strength of GB scattering can be understood by utilizing simple chemical principles. By considering the polarizability of the host atoms, we directly relate the magnitude of GB scattering to the relative degree of charge carrier screening in each material, and demonstrate that GB scattering is strongest in the ionic NaSbQ 2 -rich compounds and weakest in more polarizable PbQ-rich phases. We finally show how these chemical arguments elegantly explain the strong GB scattering in numerous other thermoelectric materials. By uniting the deleterious charge transport properties exhibited by many different compounds into a common picture, we discuss how our work gives design principles for proper microstructure engineering in emerging thermoelectric materials.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Microscale Imaging of Thermal Conductivity Suppression at Grain Boundaries

Abstract Grain‐boundary engineering is an effective strategy to tune the thermal conductivity of materials, leading to improved performance in thermoelectric, thermal‐barrier coatings, and thermal management applications. Despite the central importance to thermal transport, a clear understanding of how grain boundaries modulate the microscale heat flow is missing, owing to the scarcity of local investigations. Here, thermal imaging of individual grain boundaries is demonstrated in thermoelectric SnTe via spatially resolved frequency‐domain thermoreflectance. Measurements with microscale resolution reveal local suppressions in thermal conductivity at grain boundaries. Also, the grain‐boundary thermal resistance – extracted by employing a Gibbs excess approach – is found to be correlated with the grain‐boundary misorientation angle. Extracting thermal properties, including thermal boundary resistances, from microscale imaging can provide comprehensive understanding of how microstructure affects heat transport, crucially impacting the materials design of high‐performance thermal‐management and energy‐conversion devices.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Grain size and structure distortion characterization of α-MgAgSb thermoelectric material by powder diffraction

Nanostructuring, structure distortion and/or disorder are the main manipulation techniques to reduce the lattice thermal conductivity and improve the figure of merit of thermoelectric materials. A single-phase α-MgAgSb sample, MgAg 0.97 Sb 0.99 , with high thermoelectric performance in near room temperature region was synthesized through a high-energy ball milling with a hot-pressing method. In this work, we report the average grain size of 24-28 nm and the accurate structure distortion, which are characterized by high-resolution neutron diffraction and synchrotron X-ray diffraction with Rietveld refinement data analysis. Both the small grain size and the structure distortion have a contribution to the low lattice thermal conductivity in MgAg 0.97 Sb 0.99 .

36 MATERIALS SCIENCE↗
DOE OSTI2025

Energy filtering–induced ultrahigh thermoelectric power factors in Ni 3 Ge

Traditional thermoelectric materials rely on low thermal conductivity to enhance their efficiency but suffer from inherently limited power factors. Innovative pathways to optimize electronic transport are thus crucial. Here, we achieve ultrahigh power factors in Ni 3 Ge-based systems through an unconventional thermoelectric materials design principle. When overlapping flat and dispersive bands are engineered to the Fermi level, charge carriers can undergo intense interband scattering, yielding an energy filtering effect similar to what has long been predicted in certain nanostructured materials. Via a multistep DFT-based screening method developed here, we find a family of L1 2 -ordered binary compounds with ultrahigh power factors up to 11 mW m −1 K −2 near room temperature, which are driven by an intrinsic phonon-mediated energy filtering mechanism. Our comprehensive experimental and theoretical study of these intriguing materials paves the way for understanding and designing high-performance scattering-tuned metallic thermoelectrics.

Science & Technology - Other Topics↗
DOE OSTI2020

Ultralow thermal conductivity from transverse acoustic phonon suppression in distorted crystalline α-MgAgSb

Low thermal conductivity is favorable for preserving the temperature gradient between the two ends of a thermoelectric material, in order to ensure continuous electron current generation. In high-performance thermoelectric materials, there are two main low thermal conductivity mechanisms: the phonon anharmonic in PbTe and SnSe, and phonon scattering resulting from the dynamic disorder in AgCrSe2 and CuCrSe2, which have been successfully revealed by inelastic neutron scattering. Using neutron scattering and ab initio calculations, we report here a mechanism of static local structure distortion combined with phononanharmonic-induced ultralow lattice thermal conductivity in α-MgAgSb. Since the transverse acoustic phonons are almost fully scattered by the compound’s intrinsic distorted rocksalt sublattice, the heat is mainly transported by the longitudinal acoustic phonons. The ultralow thermal conductivity in α-MgAgSb is attributed to its atomic dynamics being altered by the structure distortion, which presents a possible microscopic route to enhance the performance of similar thermoelectric materials.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Single crystal growth and thermoelectric properties of Nowotny chimney-ladder compound Fe 2 Ge 3

Fe 2 Ge 3 with an incommensurate Nowotny chimney-ladder (NCL) structure is a promising material for thermoelectric applications due to its low thermal conductivity. Previous experimental studies on Fe 2 Ge 3 have mainly focused on polycrystalline samples, resulting in a limited understanding of the material's intrinsic thermoelectric properties and the underlying causes of its low thermal conductivity. Here we report the synthesis and thermoelectric properties of single crystalline Fe 2 Ge 3 . Millimeter-sized Fe 2 Ge 3 single crystals grown by the chemical vapor transport method enable the study of the intrinsic thermoelectric properties. The Seebeck coefficient of Fe 2 Ge 3 is negative and its magnitude increases linearly with temperature, showing a degenerate n-type semiconductor behavior. Analysis of the electrical resistivity and specific heat data indicates the existence of an Einstein mode with a characteristic temperature of about 60 K, suggesting the presence of low-energy optical phonons. Further, the thermal conductivity of Fe 2 Ge 3 along the c axis is as low as 1.9Wm -1 K -1 at 300 K and exhibits a nearly temperature-independent characteristic, which is distinct from the previous theoretical calculations with a stronger temperature dependence. The low thermal conductivity may be attributed to the scattering of acoustic phonons by low-energy optical modes and the presence of non-extended diffuson modes, as reported in another NCL compound, MnSi 1.74 . This study provides valuable insights into the electrical and thermal properties of Fe 2 Ge 3 , which can open up possibilities for future advances in thermoelectric applications.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Accelerated Discovery and Design of Ultralow Lattice Thermal Conductivity Materials Using Chemical Bonding Principles

Semiconductors with very low lattice thermal conductivities are highly desired for applications relevant to thermal energy conversion and management, such as thermoelectrics and thermal barrier coatings. Although the crystal structure and chemical bonding are known to play vital roles in shaping heat transfer behavior, material design approaches of lowering lattice thermal conductivity using chemical bonding principles are uncommon. In this work, an effective strategy of weakening interatomic interactions and therefore suppressing lattice thermal conductivity based on chemical bonding principles is presented and a high-efficiency approach of discovering low κ L materials by screening the local coordination environments of crystalline compounds is developed. The resulting first-principles calculations uncover 30 hitherto unexplored compounds with (ultra)low lattice thermal conductivities from 13 prototype crystal structures contained in the Inorganic Crystal Structure Database. Furthermore, an approach of rationally designing high-performance thermoelectrics is demonstrated by additionally incorporating cations with stereochemically active lone-pair electrons. Here these results not only provide atomic-level insights into the physical origin of the low lattice thermal conductivity in a large family of copper/silver-based compounds but also offer an efficient approach to discover and design materials with targeted thermal transport properties.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Thermomagnetic responses of semimetals

Solid-state thermomagnetic modules operating based on the Nernst–Ettingshausen effects are an alternative to conventional solid-state thermoelectric modules. These modules are appropriate for low-temperature applications where the thermoelectric modules are not efficient. Here, we briefly discuss the application, performance, similarities, and differences of thermoelectric and thermomagnetic materials and modules. We review thermomagnetic module design, Nernst coefficient measurement techniques, and theoretical advances, emphasizing the Nernst effect and factors influencing its response in semimetals such as carrier compensation, Fermi surface, mobility, phonon drag, and Berry curvature. The main objective is to summarize the materials design criteria to achieve high thermomagnetic performance to accelerate thermomagnetic materials discovery.

42 ENGINEERING↗
DOE OSTI2020

First Principle based Thermal Conductivity Modeling of Metal Alloys with Applications on Uranium Alloys

Thermal conductivity is an important materials property related to heat transport, which is essential to many applications, ranging from thermoelectrics to nuclear reactor materials. High- quality thermal conductivity data is critical to these materials and their associated technologies, including the nuclear fuel materials like traditional oxide fuels and metallic uranium (U) fuels, e.g. U-Zr and U-Mo alloys. And thermal conductivity modeling is widely used to interpolate or extrapolate experimental data, to obtain high-quality thermal conductivity data over wide temperature and composition range, and to understand the impacts of different factors including defects and microstructures. However, a general thermal conductivity model for metal alloys which can work regrading different phase components is still missing. Also, for U alloys, a thermal conductivity model working with different phases is needed. Therefore, in this work, we developed thermal conductivity models for metal alloys, based on ab-initio calculations, semi-classical physics rules, and limited experimental data. The goals of these models are to help obtain high- quality thermal conductivity data within a little experimental input as possible, have models that are extendable to varying microstructures, including different types of irradiation effects, and provide mechanistic understanding of heat transfer in the modeled alloys. In this work, our model solves several challenges in the development. The DFT-BTE approach is applied to decrease the reliance on experimental data and make the model extendable to composition changes and defects. A practical and efficient way to combine the DFT inputs with physics rules is pointed out in this work too. A staged approach, which starts from simple cases of elemental metals, then extends to solid solutions, different compound phases, and multi-phase mixtures, is presented to work with the metal alloys in different phase components. Our models are demonstrated respectively on aU for elemental metal model, on U-Zr and U-Mo alloys in aU temperature range for multi-phase mixture model, on high-temperature U-Zr, U-Nb, and U-Mo alloys in the body-centered cubic phase for concentrated solid solution model, and on irradiated U-Mo alloys for irradiated metal alloy model. All models show great agreement with experimental data. In these demonstrations, our model shows its advantages compared to previous empirical fitting model. Our model requires fewer experimental data, due to the inputs from DFT. The quantitative insights into the different physical factors are provided in our model, as it incorporates the electron and phonon scattering mechanisms. Our model also can be extended to incorporate the contributions of point defects, grain boundaries, and noble gas bubbles, to integrate their effects on heat transfer. This model can serve as both a foundation for understanding the more complex thermal conductivity of realistic U alloy fuels and a useful tool to guide further modeling of thermal conductivity to aid materials and device design.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗