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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 73 records · Page 4

Property Measurements of the NaCl-PuCl 3 Molten Salt System

Thermal properties of several compositions of the binary NaCl-PuCl 3 salt were measured to confirm the eutectic composition and provide high quality data for use by MSR developers. The PuCl 3 was generated by reducing PuO 2 to plutonium metal in the presence of calcium metal and then chlorinating the metallic plutonium with NH 4 Cl. The resulting PuCl 3 was used to make seven binary NaCl-PuCl 3 compositions with between 59.9 mol % PuCl 3 (Salt 1) and 20.0 mol % PuCl 3 (Salt 7). The eutectic temperature was measured to be 457 ± 4 °C by onset determination in DSC analyses of the seven mixtures, which is consistent with the values in the literature. Additional transitions were observed at approximately 332 and 363 °C in analyses of the PuCl 3 -rich compositions (Salts 1-3) at about 376 and 439 °C in analyses the Na-rich compositions (Salts 4-7). The solid state heat capacity decreased with increasing PuCl 3 content. The liquid state heat capacity was measured for Salt 3 (37.4 mol % PuCl 3 ) and Salt 4 (38.3 mol % PuCl 3 ). A higher heat capacity was measured for Salt 4 and measurements with both salts showed a positive correlation with temperature between 520 and 730 °C. Cells fabricated from nickel and molybdenum for use in DSC measurements at high temperatures could not be adequately sealed because these materials are not sufficiently malleable, even after high temperature annealing. It is recommended that future development focus on corrosion-resistant materials that have mechanical and thermal properties similar to the commercially available gold cells, such as Pt-Rh (80–20) and pure platinum. Those materials are chemically inert, soft, and malleable like gold, but have melting temperatures higher than 1000 °C (Rakhtsaum, 2013). Use of the Pt-Rh alloy should be evaluated first based on superior machinability for making precision parts and its current use in commercial DSC high temperature crucibles. The commercial Pt-Rh cells are not hermetically sealable, but it is expected that cells made from thinner stock can be sealed.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Non-Contact Mass Density and Thermal Conductivity Measurements of Organic Thin Films Using Frequency–Domain Thermoreflectance

Thin-film organic materials are broadly used to study amorphous stabilization of active pharmaceuticals, control explosive detonation phenomena, and introduce insulation in novel thermal barriers. Their synthesis, however, introduces defects and thickness variations that warrant careful characterization of local thermophysical properties such as thermal conductivity and mass density. In this study, wide bandwidth (200 Hz to 20 MHz) frequency–domain thermoreflectance (FDTR) is demonstrated to simultaneously extract the thermal conductivity and mass density of 1 μm physical vapor-deposited indomethacin films on Si and SiO 2 substrates, as well as 10 and 100 μm films on Si. By assuming a bulk specific heat capacity, mass densities are determined with FDTR measurements of volumetric heat capacity and are in good agreement with the literature, as well as models based upon a dependence on porosity and the kinetic theory for phonons. Lastly, it is found that for broad-band FDTR measurements, insulating substrates provide improved fidelity for the extraction of thermal conductivity and volumetric heat capacity in organic thin films. Overall, this work demonstrates the potential for FDTR as a non-contact method to determine microscale mass density variations across the surface and thickness of organic thin films.

36 MATERIALS SCIENCE↗

Generalized entanglement capacity of de Sitter space

Near horizons, quantum fields of low spin exhibit densities of states that behave asymptotically like 1 + 1 dimensional conformal field theories. In effective field theory, imposing some short-distance cutoff, one can compute thermodynamic quantities associated with the horizon, and the leading cutoff sensitivity of the heat capacity is found to equal to the leading cutoff sensitivity of the entropy. One can also compute contributions to the thermodynamic quantities from the gravitational path integral. For the cosmological horizon of the static patch of de Sitter space, a natural conjecture for the relevant heat capacity is shown to equal the Bekenstein-Hawking entropy. These observations allow us to extend the well-known notion of the generalized entropy to a generalized heat capacity for the static patch of de Sitter (dS). The finiteness of the entropy and the nonvanishing of the generalized heat capacity suggest it is useful to think about dS as a state in a finite dimensional quantum gravity model that is not maximally uncertain. Published by the American Physical Society 2024

Astronomy & Astrophysics↗

How Cooperatively Folding Are Homopolymer Molecular Knots?

Detailed thermodynamic analysis of complex systems with multiple stable configurational states allows for insight into the cooperativity of each individual transition. In this work, we derive a heat capacity decomposition comprising contributions from each individual configurational state, which together sum to a baseline heat capacity, and contributions from each state-to-state transition. We apply this analysis framework to a series of replica exchange molecular dynamics simulations of linear and 1-1 coarse-grained homo-oligomer models, which fold into stable, configurationally well-defined molecular knots, in order to better understand the parameters leading to stable and cooperative folding of these knots. We find that a stiff harmonic backbone bending angle potential is key to achieving knots with specific 3D structures. Tuning the backbone equilibrium angle in small increments yields a variety of knot topologies. Populations of different knotted states as a function of temperature can also be manipulated by tuning the backbone torsion stiffness or by adding side-chain beads. We find that sharp total heat capacity peaks for the homo-oligomer knots are largely due to a coil-to-globule transition rather than a cooperative knotting step. Furthermore, in some cases, the cooperativity of globule-to-knot and coil-to-globule transitions is comparable, suggesting that highly cooperative folding to knotted structures can be achieved by refining the model parameters or adding sequence specificity.

36 MATERIALS SCIENCE↗

Magnetic behavior of manganese chloride on Kagome and honeycomb lattices

The magnetic properties of transparent pink Na 2 Mn 3 Cl 8 and NaMnCl3 are presented. For both phases, the effective magnetic moments are large, while the Curie-Weiss thetas are below 10 K. The compounds crystallize in the trigonal R-3m and R-3 space groups, respectively. A Kagome plane of Mn 2+ octahedrally coordinated to Cl- is found in Na 2 Mn 3 Cl 8 and the material has no apparent magnetic ordering above 1.8 K, while the octahedrally coordinated, honeycomb network of Mn 2+ in NaMnCl 3 orders antiferromagnetically at 6.3 ± 0.2 K. The heat capacity of NaMnCl3 has one transition, consistent with the susceptibility, while Na 2 Mn 3 Cl 8 exhibits a more complex heat capacity with two peaks, at 0.6 K and 1.4 K. A third, broad peak near 6.2 K in the heat capacity of Na 2 Mn 3 Cl 8 is problematic but may be due to the intergrowth of NaMnCl 3 domains.

36 MATERIALS SCIENCE↗

Stripe antiferromagnetic ground state of the ideal triangular lattice compound KErSe 2

Rare-earth triangular lattice materials have been proposed as a good platform for the investigation of frustrated magnetic ground states. KErSe 2 , with the delafossite structure, contains perfect two-dimensional Er 3 + triangular layers separated by potassium ions, realizing this ideal configuration and inviting study. In this study, we investigate the magnetism of KErSe 2 at millikelvin temperatures by heat capacity and neutron powder diffraction. Heat capacity results reveal a magnetic transition at 0.2 K in zero applied field. This long-range order is suppressed by an applied magnetic field of 0.5 T below 0.08 K. Neutron powder diffraction suggests that the zero-field magnetic structure orders with k = ( 1 2 , 0 , 1 2 ) in a stripe spin structure. Unexpectedly, Er is found to have a reduced moment of 3.06(1) μ B /Er in the ordered state, and diffuse magnetic scattering, which originates at higher temperatures, is found to persist in the ordered state, potentially indicating magnetic fluctuations. Neutron diffraction collected under an applied field shows a metamagnetic transition at ~ 0.5 T to ferromagnetic order with k = ( 0 , 0 , 0 ) and two possible structures, which are likely dependent on the applied field direction. The zero-field stripe spin structure can be explained by the anisotropic interactions or the first-, second-, and third-neighbor couplings in the antiferromagnetic triangular lattice.

2-dimensional systems↗

Disorder-induced local strain distribution in Y-substituted TmVO 4

We report an investigation of the effect of substitution of Y for Tm in Tm 1-x ⁢Y x VO 4 via low-temperature heat capacity measurements, with the yttrium content x varying from 0 to 0.997. Because the Tm ions support a local quadrupolar (nematic) moment, they act as reporters of the local strain state in the material, with the splitting of the ion's non-Kramers crystal field ground state proportional to the quadrature sum of the in-plane tetragonal symmetry-breaking transverse and longitudinal strains experienced by each ion individually. Analysis of the heat capacity, therefore, provides detailed insights into the distribution of local strains that arise as a consequence of the chemical substitution. These local strains suppress long-range quadrupole order for x > 0.22, and result in a broad Schottky-like feature for higher concentrations. Heat capacity data are compared to expectations for a distribution of uncorrelated (random) strains. For dilute Tm concentrations, the heat capacity cannot be accounted for by randomly distributed strains, demonstrating the presence of significant strain correlations between sites. For intermediate Tm concentrations, these correlations must still exist, but the data cannot be distinguished from that which would be obtained from a two-dimensional Gaussian distribution. The crossover between these limits is discussed in terms of the interplay of key lengthscales in the substituted material. Furthermore, the central result of this work, namely that local strains arising from chemical substitution are not uncorrelated, has implications for the range of validity of theoretical models based on random effective fields that are used to describe such chemically substituted materials, particularly when electronic nematic correlations are present.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Large magnetoresistance and first-order phase transition in antiferromagnetic single-crystalline EuAg 4 Sb 2

Here, we present the results of a thorough investigation of the physical properties of EuAg 4 Sb 2 single crystals using magnetization, heat capacity, and electrical resistivity measurements. High-quality single crystals, which crystallize in a trigonal structure with space group 𝑅⁢$\bar{3}$𝑚, were grown using a conventional flux method. Temperature-dependent magnetization measurements along different crystallographic orientations confirm two antiferromagnetic phase transitions around 𝑇 𝑁⁢1 = 10.5K and 𝑇 𝑁⁢2 = 7.5K. Isothermal magnetization data exhibit several metamagnetic transitions below these transition temperatures. Antiferromagnetic phase transitions in EuAg 4 Sb 2 are further confirmed by two sharp peaks in the temperature-dependent heat capacity data at 𝑇 𝑁⁢1 and 𝑇 𝑁⁢2 , which shift to lower temperature in the presence of an external magnetic field. Our systematic heat capacity measurements utilizing a long-pulse and single-slope analysis technique allow us to detect a first-order phase transition in EuAg 4 Sb 2 at 7.5 K. The temperature-dependent electrical resistivity data also manifest two features associated with magnetic order. The magnetoresistance exhibits a broad hump due to a field-induced metamagnetic transition. Remarkably, the magnetoresistance keeps increasing without showing any tendency to saturate as the applied magnetic field increases, and it reaches ∼20 000% at 1.6 K and 60 T. At high magnetic fields, several magnetic quantum oscillations are observed, indicating a complex Fermi surface. A large negative magnetoresistance of about −55% is also observed near 𝑇 𝑁⁢1 . Moreover, the 𝐻−𝑇 phase diagram constructed using magnetization, heat capacity, and magnetotransport data indicates complex magnetic behavior in EuAg 4 Sb 2 .

36 MATERIALS SCIENCE↗

Property Measurements of NaCl-UCl 3 and LiF-NaF-KF Molten Salts Doped with Surrogate Fission Products

Knowing thermophysical and thermochemical property values of salts over the expected range of operating temperatures is essential to modeling and simulation efforts that support the commercialization of molten salt reactor (MSR) technologies. Salt properties being measured at Argonne include thermal transitions, phase behavior, heat capacity, density, surface tension, volumetric thermal expansion, thermal diffusivity, thermal conductivity, and viscosity. The properties of several salts of interest including NaCl-UCl 3 and LiF-NaF-KF (FLiNaK) have been measured at Argonne and reported previously. These property measurements are suitable for use in evaluating reactor performance during startup and the early operating life of the reactor. The physical and chemical behavior of the fuel salt is altered by the buildup of fission products and the resulting changes in heat transfer and other properties must be understood by reactor developers. This report summarizes melting behavior, heat capacity, and thermal diffusivity values that were measured for mixtures of FLiNaK and NaCl-UCl 3 salts that have been doped with surrogate fission products. Additional heat capacity measurements were also performed on a separate mixture of FLiNaK without dopants. Measured properties are suitable for incorporation into the Molten Salt Thermal Properties Database–Thermochemical (MSTDB–TC) and the Molten Salt Thermal Properties Database–Thermophysical (MSTDB–TP) to support the development of MSRs. Salts were prepared by doping eutectic mixtures of NaCl-UCl 3 and FLiNaK with surrogate fission products. These salts were prepared for use in salt spill experiments being performed at Argonne and were subsequently used for thermal property measurements. Thermal transitions and heat capacities were measured by using differential scanning calorimetry (DSC) and thermal diffusivity was measured by using laser flash analysis (LFA) at temperatures spanning the typical MSR operating range. The measured property values of the doped salts were compared to measured property values of salts without fission products to quantify the effects of the doped fission products.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

High‑performance cold‑climate heat pump using tandem compressors with and without vapor injection: Laboratory investigation and field demonstration

Cold‑climate air‑source heat pumps must maintain heating capacity and stable operation at low ambient temperatures for residential applications. This study adapts tandem single-speed compressors—proven in commercial systems —for residential CCHPs, integrating VI and validating performance across laboratory and extreme field conditions to achieve cold-climate targets. That is to achieve ≥75% of the rated heating capacity at −25.0 °C relative to 8.3 °C and heating coefficient of performance (COP) greater than 4.0 at 8.3 °C. Laboratory testing confirmed that both configurations met these targets while operating within acceptable discharge‑temperature limits. Relative to the non‑VI configuration, the VI system provided up to 15% higher heating capacity and up to 9% higher heating COP under identical conditions, yielding a 5.6–9.1% increase in heating seasonal performance factor (HSPF). Field tests in Ohio and Alaska, with minimum outdoor temperatures of −25.0 °C and −34.0 °C, respectively, showed stable operation, minimal supplemental heating (<3.2%), low defrost penalties, and consistent output. Tandem‑compressor architectures proves promising for cold-climate residential heating.

Hu, Yifeng [ORNL] (ORCID:0000000242875185)↗

Using Hyperoptimized Tensor Networks and First-Principles Electronic Structure to Simulate the Experimental Properties of the Giant {Mn 84 } Torus

The single-molecule magnet {Mn 84 } is a challenge to theory because of its high nuclearity. Here, we directly compute two experimentally accessible observables, the field-dependent magnetization up to 75 T and the temperature-dependent heat capacity, using parameter-free theory. In particular, we use first-principles calculations to derive short- and long-range exchange interactions and compute the exact partition function of the resulting classical Potts and Ising spin models for all 84 Mn S = 2 spins to obtain observables. The latter computation is made possible by using hyperoptimized tensor network contractions, a technique developed to simulate quantum supremacy circuits. We also synthesize the magnet and measure its heat capacity and magnetization, observing qualitative agreement between theory and experiment and identifying an unusual bump in the heat capacity and a plateau in the magnetization. Our work also identifies some limitations of current theoretical modeling in large magnets, such as sensitivity to small, long-range exchange couplings.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Thermodynamic stability and contributions to the Gibbs free energy of nanocrystalline Ni 3 Fe

In this work, the heat capacities of nanocrystalline Ni 3 Fe and control materials with larger crystallites were measured from 0.4–300 K. The heat capacities were integrated to obtain the enthalpy, entropy, and Gibbs free energy and to quantify how these thermodynamic functions are altered by nanocrystallinity. From the phonon density of states (DOS) measured by inelastic neutron scattering, we find that the Gibbs free energy is dominated by phonons and that the larger heat capacity of the nanomaterial below 100 K is attributable to its enhanced phonon DOS at low energies. Besides electronic and magnetic contributions, the nanocrystalline material has an additional contribution at higher temperatures, consistent with phonon anharmonicity. The nanocrystalline material shows a stronger increase with temperature of both the enthalpy and entropy compared to the bulk sample. Its entropy exceeds that of the bulk material by 0.4 $k_B$/atom at 300 K. This is insufficient to overcome the enthalpy of grain boundaries and defects in the nanocrystalline material, making it thermodynamically unstable with respect to the bulk control material.

36 MATERIALS SCIENCE↗

Superconductivity by alloying the topological insulator SnBi 2 Te 4

Alloying indium into the topological insulator SnBi 2 Te 4 induces bulk superconductivity with critical temperatures T c up to 1.85 K and upper critical fields up to about 14 kOe. This is confirmed by electrical resistivity, heat capacity, and magnetic susceptibility measurements. The heat capacity shows a discontinuity at T c and temperature dependence below T c consistent with weak coupling BCS theory, and suggests a superconducting gap near 0.25 meV. The superconductivity is type-II and the topological surface states have been verified by photoemission. Here, a simple picture suggests analogies with the isostructural magnetic topological insulator MnBi 2 Te 4 , in which a natural heterostructure hosts complementary properties on different sublattices, and motivates new interest in this large family of compounds. The existence of both topological surface states and superconductivity in Sn 1-x In x Bi 2 Te 4 identifies these materials as promising candidates for the study of topological superconductivity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Impact of neutron irradiation on the thermophysical properties of additively manufactured stainless steel and inconel

The deployment of additive manufacturing (AM) technologies to support the nuclear energy industry is limited by the current lack of data related to the irradiation performance of AM parts. The Colorado School of Mines is conducting a multi-year irradiation and post irradiation examination project to study the impacts of neutron irradiation on stainless steel 316L and Inconel 718 and 625 specimens produced by several commercially available AM techniques and irradiated in the Advanced Test Reactor (ATR) at the Idaho National Laboratory (INL). This paper presents initial results on the impact of neutron irradiation on the heat capacity, the thermal diffusivity, and the thermal conductivity of the specimens at temperatures between 100 oC and 400 oC. The unirradiated AM specimens have heat capacity values similar to, or lower than, the reference values, regardless of manufacturing method or material. The irradiated AM specimens have average heat capacities greater than the unirradiated specimens and reference values in every case. Additionally, the thermal diffusivities of the unirradiated AM specimens are either larger or statistically similar to the reference values. The irradiated AM specimens exhibit lower thermal diffusivities compared to the reference thermal diffusivity values. One of the stainless steel 316L laser powder bed fusion samples exhibited thermal diffusivity values with statistically significant anisotropy prior to and after irradiation. The thermal conductivities of the unirradiated AM stainless steel 316L specimens and the unirradiated Inconel 718 specimens are lower or statistically similar to the reference values. The unirradiated Inconel 625 specimens exhibit slightly higher thermal conductivity values than the reference values. The irradiated specimens show a significant increase in thermal conductivity compared to the unirradiated specimens and the reference values for all materials.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Thermodynamics of the Nonrelativistic Free-Electron Fermi Gas in One, Two, and Three Dimensions from the Degenerate to the Nondegenerate Temperature Regime

The thermodynamic properties of a nonrelativistic free-electron Fermi gas is of fundamental interest in condensed matter physics. Properties previously studied in three-dimensions (3D) in the lowand high-temperature limits include the internal energy, heat capacity, zero-field magnetic spin susceptibility, and pressure. Here we report solutions for the temperature dependence spanning these two temperature regimes of the chemical potential, internal energy, magnetic susceptibility, and the heat capacity at constant volume in 1D, 2D, and 3D. Also calculated are the pressure, enthalpy, heat capacity at constant pressure, isothermal compressibility, and thermal expansion coefficient versus temperature in 2D and 3D. Of primary interest here are the detailed dimension-dependent crossovers of these properties between the degenerate and nondegenerate temperature regime, which are graphically illustrated for each of the above properties.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Magnetic ground state of La 2 LiMoO 6 : A comparison with other Mo 5+ ( S=1/2 ) double perovskites

La 2 LiMoO 6 is a double perovskite (DP) with P2 1 /n symmetry based on the Mo5+ ion, 4d1, t2g1, S=1/2. It is isostructural with Sr 2 YMoO 6 , the magnetic ground state of which is apparently a very unusual collective spin singlet or valence-bond glass state as is the case for cubic (Fm-3m) Ba 2 YMoO 6 . Initial studies of La 2 LiMoO 6 suggested a different ground state from the other DPs but no clear conclusions could be drawn. A more detailed study is presented here including magnetic susceptibility, heat capacity, and elastic neutron-scattering results. This DP is now well characterized as an antiferromagnet, T N =18K, via observation of magnetic Bragg peaks in neutron scattering and an anomaly in the magnetic heat capacity. The ordering wave vector is k=( 1/21/2 0), consistent with a type I face-centered-cubic magnetic structure, and the ordered moment on Mo 5+ is 0.32(11)μ B , much reduced from the spin-only value of 1μ B . The index, f=|v c |/T N ~3, indicates a low level of frustration. The heat-capacity data above T N can be interpreted in terms of a one-dimensional spin-correlation model, as can the low-temperature data which follow a T 1 power law. This is consistent with an earlier suggestion. The difference with isostructural Sr 2 YMoO 6 is attributed to differences in the local distortion of the Mo–O octahedron and the resulting orbital ordering.

36 MATERIALS SCIENCE↗

Evaluation of measuring thermal conductivity of isotropic and anisotropic thermally insulating materials by transient plane source (Hot Disk) technique

The transient plane source (TPS) technique, also referred as the Hot Disk method, has been widely used due to its ability to measure the thermal properties of an extensive range of materials (solids, liquids, and powder). Recently, it has been recognized that typical Hot Disk sensors can influence TPS results of thermally insulating materials and lead to an overestimation of thermal conductivity. Although improvements have been proposed, they have not yet been implemented in the commercial TPS, leaving researchers with non-standardized modifications or options provided by a commercial Hot Disk apparatus. An empirical study of thermally insulating materials such as extruded polystyrene (XPS) and aerogel blanket is conducted in order to address the factors that affect the reliability of thermal conductivity k obtained using the commercial TPS apparatus. Sensor size, input power, duration of the measurements, applied pressure, and, in the case of anisotropic materials, heat capacity are investigated, and the results are compared with those using a Heat Flow Meter apparatus. The effect of sensor size on the k value is ascribed to heat loss through connecting leads and is more pronounced in smaller sensors and in materials with lower k values . In the case of XPS and aerogel, the effect becomes minimal for sensors with a radius r ≥ 6.4 mm. The low input power yields a high scattering of the results and should be avoided. Applied contact pressure and the tested region of the specimen play an important role in experiments with low-density fibrous materials due to the large percentage of heat being transferred by radiation and the heterogeneous nature of the samples, respectively. Additionally, the sensitivity of anisotropic measurements to the value of the material’s volumetric heat capacity ( ρC p ) is shown, emphasizing the need for the precise determination.

thermal conductivity↗

Heating performance of a vapor compression heat pump cascaded with a thermoelectric heat pump

Air source heat pumps (ASHPs) are widely utilized for heating and cooling in residential buildings; however, their effectiveness in heating mode is compromised during extreme weather conditions. Extensive research endeavors have been undertaken to develop, test, and assess a cost-effective vapor compression ASHP suitable for cold climate regions. Further, this study takes an innovative approach by developing component and system prototypes for a cold climate heat pump. This design combines a thermoelectric heat pump (TEHP) with a traditional residential split ASHP to augment heating capacity in low ambient temperature conditions. The component and system prototypes underwent experimental testing in the psychrometric chambers. The experimental findings revealed a 13.6% to 13.7% increase in total heat pump heating capacity, accompanied by a 3.1% to 5.0% decrease in the coefficient of performance (COP) at ambient temperatures of -15°C and -19°C, when compared to the original ASHP. The COP of the TEHP is relatively constant, ranging from 1.63 to 1.76. This prototype offers a solution to address the challenges associated with reduced heat pump capacity at low ambient temperatures. The experimental results indicated that the lower the ambient temperature, thermoelectric heat pump auxiliary heating can increase the heating efficiency 60% in comparison to electric resistance.

42 ENGINEERING↗