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DOE OSTI2019

Determination of Thermodynamic Properties of Si-B Alloys

This study establishes the thermodynamic properties of the Si-B binary alloy system. The electromotive force (emf) as a function of temperature (823 K to 923 K) was measured using solid-state electrochemical cells, represented as(−) Pt,Ar/{Si∥CaF_2∥} {Si−B(alloy)}/Ar,Pt(+) Using the experimental emf data obtained from the solid-state heterogeneous phase equilibrium, the activities of Si and B in Si-B alloys were calculated. The integral Gibbs energy of mixing (ΔG{sup M}) of alloys were calculated from the activity of Si and B. A large negative deviation from ideality was found for the integral Gibbs energy of mixing (ΔG{sup M}) of the binary Si-B system. From the activities of Si and B, the Gibbs energies of formation (ΔG{sub f}{sup 0}) of phases present were calculated. The ΔG{sub f}{sup 0} of SiB{sub 3}, the most thermodynamically stable phase, was calculated as − 13.13 ± 0.19 kJ/mole-atoms at 923 K. The heterogeneous phases and microstructure after the equilibrium study of the electrode were characterized using XRD, SEM, and EDS analyses.

36 MATERIALS SCIENCE↗

DOE OSTI2019

Oxygen Potential of High-Titania Slag from the Smelting Process of Ilmenite

Oxygen potential of TiO{sub 2}-FeO-Ti{sub 2}O{sub 3} ternary slags was determined by the electromotive force (EMF) method based on the solid electrolyte oxygen sensor at 2003 K (1730 °C). The effect of FeO content and Ti{sup 3+}/Ti{sup 4+} mass ratio on the oxygen potential of the high-titania slag was also studied. At a fixed Ti{sup 3+}/Ti{sup 4+} mass ratio of 3.11, the oxygen potential increased with increasing FeO content. Increase of Ti{sup 3+}/Ti{sup 4+} mass ratio from 2.29 to 3.60 caused a significant decrease in the oxygen potential of the slag. Comparing measured oxygen potential with the calculated values indicated that the oxygen potential of the slag might be determined by FeO/Fe equilibrium reaction rather than TiO{sub 2}/Ti{sub 2}O{sub 3} reaction. In addition, the experimentally measured oxygen potential values were modeled by multiple linear regression analysis, and a semi-empirical mathematical correlation was established between the oxygen potential and slag compositions. The iso-oxygen potential distribution diagram based on the mathematical model was obtained for the high-titania slag.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Application of the Solute-Solvent EMF Cell to Measure Activity of NiF 2 in Molten FLiNaK

Electromotive force (emf) measurements made using a combination of solute- and solvent-based electrodes were used to determine the activity of NiF 2 in molten FLiNaK eutectic at 823 K across a concentration range of x NiF2 = 5.2 × 10 –4 –1.0 × 10 –2 . The solute emf values were measured using electrodes consisting of Ni wires immersed in FLiNaK with dissolved NiF 2 contained in graphite crucibles. The measured emf values were then converted to the FLiNaK Eutectic Potassium Electrode (FEKE) potential and used to quantify the activity of dissolved NiF 2 . This quantification was based upon comparative measurements of a reference solvent electrode consisting of a K-Bi alloy immersed in pure FLiNaK contained in a boron nitride crucible and a solute electrode. Short cell lives were characteristic of the measurements due to the corrosive nature of the fluoride salts. Quantifying the activity of NiF 2 will improve the utility of Ni 2+ /Ni reference electrodes in molten fluoride salts, which are notoriously difficult electrolytes to work with because of their reactivity. In conclusion, this work demonstrates the general nature of the solute-solvent approach as a repeatable, easily employed method for measuring the activity values of electroactive species in a variety of molten salts to improve understanding of the electroactive species behavior in these systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2014

Effects of anisotropies in turbulent magnetic diffusion in mean-field solar dynamo models

We study how anisotropies of turbulent diffusion affect the evolution of large-scale magnetic fields and the dynamo process on the Sun. The effect of anisotropy is calculated in a mean-field magnetohydrodynamics framework assuming that triple correlations provide relaxation to the turbulent electromotive force (so-called the 'minimal τ-approximation'). We examine two types of mean-field dynamo models: the well-known benchmark flux-transport model and a distributed-dynamo model with a subsurface rotational shear layer. For both models, we investigate effects of the double- and triple-cell meridional circulation, recently suggested by helioseismology and numerical simulations. To characterize the anisotropy effects, we introduce a parameter of anisotropy as a ratio of the radial and horizontal intensities of turbulent mixing. It is found that the anisotropy affects the distribution of magnetic fields inside the convection zone. The concentration of the magnetic flux near the bottom and top boundaries of the convection zone is greater when the anisotropy is stronger. It is shown that the critical dynamo number and the dynamo period approach to constant values for large values of the anisotropy parameter. The anisotropy reduces the overlap of toroidal magnetic fields generated in subsequent dynamo cycles, in the time-latitude 'butterfly' diagram. If we assume that sunspots are formed in the vicinity of the subsurface shear layer, then the distributed dynamo model with the anisotropic diffusivity satisfies the observational constraints from helioseismology and is consistent with the value of effective turbulent diffusion estimated from the dynamics of surface magnetic fields.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2016

A NEW SIMPLE DYNAMO MODEL FOR STELLAR ACTIVITY CYCLE

A new simple dynamo model for stellar activity cycle is proposed. By considering an inhomogeneous flow effect on turbulence, it is shown that turbulent cross helicity (velocity–magnetic-field correlation) enters the expression of turbulent electromotive force as the coupling coefficient for the mean absolute vorticity. This makes the present model different from the current α –Ω-type models in two main ways. First, in addition to the usual helicity ( α ) and turbulent magnetic diffusivity ( β ) effects, we consider the cross-helicity effect as a key ingredient of the dynamo process. Second, the spatiotemporal evolution of cross helicity is solved simultaneously with the mean magnetic fields. The basic scenario is as follows. In the presence of turbulent cross helicity, the toroidal field is induced by the toroidal rotation. Then, as in usual models, the α effect generates the poloidal field from the toroidal one. This induced poloidal field produces a turbulent cross helicity whose sign is opposite to the original one (negative production). With this cross helicity of the reversed sign, a reversal in field configuration starts. Eigenvalue analyses of the simplest possible model give a butterfly diagram, which confirms the above scenario and the equatorward migrations, the phase relationship between the cross helicity and magnetic fields. These results suggest that the oscillation of the turbulent cross helicity is a key for the activity cycle. The reversal of the cross helicity is not the result of the magnetic-field reversal, but the cause of the latter. This new model is expected to open up the possibility of the mean-field or turbulence closure dynamo approaches.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2026

Understanding Large-Scale Dynamos in Unstratified Rotating Shear Flows

For this work, we combine simulations with new analyses that overcome previous pitfalls to explicate how nonhelical mean-field dynamos grow and saturate in unstratified, magnetorotationally driven turbulence. Shear of the mean radial magnetic field amplifies the azimuthal component. Radial fields are regenerated by velocity fluctuations that induce shear of radial magnetic fluctuations, followed by Lorentz and Coriolis forces that source a negative off-diagonal component in the turbulent diffusivity tensor. We present a simple schematic to illustrate this dynamo growth. A different part of the Lorentz force forms a third-order correlator in the mean electromotive force that saturates the dynamo.

accretion disk & black-hole plasma↗

DOE OSTI2014

Bimodular high temperature planar oxygen gas sensor

A bimodular planar O 2 sensor was fabricated using NiO nanoparticles (NPs) thin film coated yttria-stabilized zirconia (YSZ) substrate. The thin film was prepared by radio frequency (r.f.) magnetron sputtering of NiO on YSZ substrate, followed by high temperature sintering. The surface morphology of NiO NPs film was characterized by atomic force microscope (AFM) and scanning electron microscope (SEM). X-ray diffraction (XRD) patterns of NiO NPs thin film before and after high temperature O 2 sensing demonstrated that the sensing material possesses a good chemical and structure stability. The oxygen detection experiments were performed at 500, 600, and 800°C using the as-prepared bimodular O 2 sensor under both potentiometric and resistance modules. For the potentiometric module, a linear relationship between electromotive force (EMF) output of the sensor and the logarithm of O 2 concentration was observed at each operating temperature, following the Nernst law. For the resistance module, the logarithm of electrical conductivity was proportional to the logarithm of oxygen concentration at each operating temperature, in good agreement with literature report. In addition, this bimodular sensor shows sensitive, reproducible and reversible response to oxygen under both sensing modules. Integration of two sensing modules into one sensor could greatly enrich the information output and would open a new venue in the development of high temperature gas sensors.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Combined Experimental and Computational Study of Molybdenum and Niobium for Nuclear Sensor Application

Due to their novel electromagnetic and thermal properties, molybdenum (Mo) and niobium (Nb) become optimal temperature sensor materials for nuclear energy applications. We leveraged voltage recorded during a heat ramp to tune a computational method to predict the Seebeck electromotive force (EMF) of Mo and Nb. Using a combined Density Functional Theory (DFT) and Boltzmann Transport Equations (BTE) method the voltage was predicted but did not include the effects of temperature on atomic structure. Combining Ab Initio Molecular Dynamics (AIMD) and BTE included temperature effects on structure optimization and yielded voltages in a good agreement with experiment. Lanthanum (La) and Phosphorus (P) additives in Mo and Nb, respectively, could increase the EMF compared to those of the pure metals. The presence of oxygen (O) in Mo increases the EMF while O in Nb slightly reduces the EMF. Furthermore, our studies suggested that heat treatment-induced structural changes that lead to a reduction in voltage occur not only at the mesoscale as previously understood but also at the atomic scale.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2021

Thermodynamic properties of the Nd-Bi system via emf measurements, $\mathrm{DFT}$ calculations, machine learning, and $\mathrm{CALPHAD}$ modeling

Thermodynamic properties of the Nd-Bi system were investigated using a combination of experimental measurements, first-principles calculations based on density functional theory (DFT), data mining and machine learning (DM + ML) predictions, and calculation of phase diagrams (CALPHAD) modeling. The electromotive force (emf) of Nd-Bi alloys in molten LiCl-KCl-NdCl 3 at 773–973 K was measured via coulometric titration of Nd into Bi for the determination of thermochemical properties such as activity coefficients and solubilities of Nd in Bi. A new peritectic reaction of [liquid + NdBi 2 = Nd 3 Bi 7 ] at 774 K was confirmed using differential scanning calorimetry, structural (X-ray diffraction), and microstructural (scanning electron microscopy) analyses. The unknown crystal structure of NdBi2 was suggested to be a mixture of the anti-La 2 Sb configuration and the La 2 Te-type configuration based on ML predictions for over 26,000 data-mined AB 2 -type configurations together with DFT-based verifications. Using the newly acquired experimental data and DFT-based calculations, the thermodynamic description of the Nd-Bi system was remodeled, and a more complete Nd-Bi phase diagram was calculated, including the Nd 3 Bi 7 compound, invariant transition reactions, and liquidus temperatures.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Fabrication of highly dense isotropic Nd-Fe-B nylon bonded magnets via extrusion-based additive manufacturing [Fabrication of highly dense isotropic Nd-Fe-B bonded magnets via extrusion-based additive manufacturing]

Magnetically isotropic bonded magnets with a high loading fraction of 70 vol.% Nd-Fe-B are fabricated via an extrusion-based additive manufacturing, or 3D printing system that enables rapid production of large parts. The density of the printed magnet is ~5.2 g/cm 3 . The room temperature magnetic properties are: intrinsic coercivity H ci = 8.9 kOe (708.2 kA/m), remanence B r = 5.8 kG (0.58 T), and energy product (BH)max = 7.3 MGOe (58.1 kJ/m 3 ). The as-printed magnets are then coated with two types of polymers, both of which improve the thermal stability as revealed by flux aging loss measurements. Tensile tests performed at 25 °C and 100 °C show that the ultimate tensile stress (UTS) increases with increasing loading fraction of the magnet powder, and decreases with increasing temperature. AC magnetic susceptibility and resistivity measurements show that the 3D printed Nd-Fe-B bonded magnets exhibit extremely low eddy current loss and high resistivity. Lastly, we demonstrate the performance of the 3D printed magnets in a DC motor configuration via back electromotive force measurements.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Stable perovskite-fluorite dual-phase composites synthesized by one-pot solid-state reactive sintering for protonic ceramic fuel cells

We report that this work synthesized a series of oxide composites with nominal compositions of BaCe 05 Zr 0.4 Y 0.1 O 3-δ (BCZY)-Ce 0.5 Y 0.5 O 2-δ (YDC) based on the BCZY/YDC molar ratios of 0.5:1, 1:1, 2:1, and 4:1 (BCZY-YDC-0.5–1, BCZY-YDC-1-1, BCZY-YDC-2-1, and BCZY-YDC-4-1) using a one-pot solid state reactive sintering (SSRS) method. The X-ray diffraction (XRD) patterns and refinement proved that the one-pot SSRS at 1450 °C for 12 h could achieve the perovskite-fluorite dual-phase composites (DPCs) with the desired structure compositions. The scanning electron microscopy (SEM) images showed that the two DPCs of BCZY-YDC-1-1 and BCZY-YDC-2-1 formed excellent percolation for perovskite and fluorite phases. The conductivity measurement by electrochemical impedance spectroscopy (EIS) and the transference number measurement by the electromotive force (EMF) test proved that changing the BCZY/YDC molar ratio and operating condition could adjust the DPC's conduction property to make them suitable for electrolytes and electrode scaffolds for protonic ceramic fuel cells (PCFCs). The long-term conductivity testing and the crystal structure analysis after EMF testing under versatile conditions indicated that the DPCs of BCZY-YDC-2-1 and BCZY-YDC-1-1 were durable PCFC component materials. The PCFC button cells with the as-discovered BCZY-YDC-2-1 and BCZY-YDC-1-1 as an electrolyte and an anode scaffold, respectively, and the reported Ba–Ce–Fe–Co–O perovskite-perovskite composite as a cathode showed promising performance under H 2 /air gradient.

08 HYDROGEN↗

DOE OSTI2021

Thermodynamic properties of Gd-Bi alloys determined by emf measurements in LiCl-KCl-GdCl 3 electrolyte

Thermodynamic properties of binary Gd-Bi alloys (mole fraction, x Gd = 0.02–0.35) were determined using electromotive force (emf) measurements in molten LiCl-KCl-GdCl 3 electrolyte in complement with structural, microstructural, and thermal characterization. X-ray diffractometry (XRD) and scanning electron microscopy (SEM) identified the phase constituents of Gd-Bi alloys (x Gd = 0.02–0.35) as Bi matrix and GdBi compound. According to differential scanning calorimetry (DSC) measurements up to 1250 K, a eutectic transition [L = Bi + GdBi] was observed at 543 K but the reported peritectic transition [L + GdBi = GdBi 2 ] was not detected, suggesting the absence of the GdBi 2 compound. Based on structural, microstructural, and thermal characterization of Gd-Bi alloys (x Gd = 0.02–0.35), the GdBi 2 compound was not detected, and its thermodynamic stability is questionable. The emf of Gd-Bi alloy (x Gd = 0.16) at 700–1048 K relative to Gd(s) was measured by electrodepositing pure Gd metal at 25 K increments. Further, the emf values of Gd-Bi alloys were determined via coulometric titration of Gd into liquid Bi using a two-phase [L + GdBi] alloy as a reference electrode at 773–973 K. The solubility of Gd in liquid Bi was also estimated to be 0.50 mol% (773 K), 0.99 mol% (873 K), and 2.21 mol% (973 K) and the excess partial molar Gibbs energy (Δ$\mathrm{\bar{G}^{ex}_{Gd}}$) of liquid Gd-Bi alloys was as low as 65 kJ mol –1 , indicating strong chemical interactions between Gd and Bi.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Thermoelectrics: From longitudinal to transverse

Thermoelectric power generation is a promising technology to realize a sustainable society because it directly converts thermal energy into electricity in a solid. Conventional thermoelectric generation is driven by the Seebeck effect, discovered by T.J. Seebeck in 1821, in which a charge current J c is generated in the direction parallel to a temperature gradient ∇T, the longitudinal geometry. Here, the ratio between the generated longitudinal electromotive force and applied ∇T is defined as the Seebeck coefficient. As shown in Figure 1A, a thermoelectric module based on the Seebeck effect typically consists of many pairs (128 for a 12V unit) of p-type and n-type conductors alternately arranged and connected in series. Since the Seebeck coefficient of a p-type (n-type) conductor is positive (negative), the thermopower in each element adds to the total output in the Seebeck module. This configuration is needed to achieve a practical voltage because each element only supplies millivolts but limits the use of thermoelectric generators. The efficiency of thermoelectric generators is characterized by the thermoelectric figure of merit, zT. Despite a 3-fold improvement in zT resulting from materials research over the last two decades, little progress has been made in their practical use; this is ascribed to the technological challenges in contact technology. The contacts on the hot side are subject to thermal degradation. All contacts (512 for a 12V unit) add electrical and thermal contact resistances that reduce the device efficiency to a fraction of that promised by the materials.

30 DIRECT ENERGY CONVERSION↗

DOE OSTI2020

Hydroxypyridinone-based stabilization of Np(IV) enabling efficient U/Np/Pu separations in the Adapted PUREX process

The classical process to recover uranium (U) and plutonium (Pu) from used nuclear fuel using tributyl phosphate (TBP), namely the Plutonium Uranium Redox EXtraction (PUREX) process, is complicated by the persistent presence of neptunium (Np) and thus requires extra purification steps. The concept of Adapted PUREX seeks to achieve Np recovery by adjusting the valence of the metal more effectively, thereby controlling its behavior more precisely. This study introduces the use of an aqueous hydroxypyridinone chelator, 3,4,3-LI(1,2-HOPO) (abbreviated as HOPO), to dictate the behavior of Np for recovery and meanwhile simplify cumbersome reprocessing steps. The interactions between Np and HOPO were probed mechanistically by way of absorption spectrophotometry, in conjunction with cyclic voltammetry. UV–Vis-NIR spectra illustrated the reduction of NpO 2 2+ to Np 4+ , with a fast reaction rate. Cyclic voltammetry revealed quasi-reversible processes between the oxidized and reduced forms of the ligand and its Np complexes. The corresponding heterogeneous rate constants (k 0 ) were estimated from the peak-to-peak separation potentials (ΔE p ), at ~ 4 – 35 μm/s for both HOPO and NpHOPO, with scan rates of 0.01 – 0.4 V/s. Meanwhile, the electromotive force (E MF ) as well as the change of Gibbs free energy (ΔG) were assessed from the half-wave potential (E 1/2 ), demonstrating the completeness of NpO 2 2+ reduction to Np 4+ by HOPO. The cumulative formation constant of the resulting NpHOPO complex (logβ 101 ) was determined by metal competition titration to be 42.0 ± 0.6, corroborating the extraordinarily high affinity of HOPO to tetravalent metal ions. Here, the prowess of valence control by HOPO and the high stability of the formed complex resulted in enhanced separations of Np from U and of Pu from U, with a maximum separation factor of ~7000 for both, nearly 90- and 10300-fold higher, respectively, than the values obtained using conventional PUREX formulae.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2016

The magnetic shear-current effect: Generation of large-scale magnetic fields by the small-scale dynamo

A novel large-scale dynamo mechanism, the magnetic shear-current effect, is discussed and explored. Here, the effect relies on the interaction of magnetic fluctuations with a mean shear flow, meaning the saturated state of the small-scale dynamo can drive a large-scale dynamo – in some sense the inverse of dynamo quenching. The dynamo is non-helical, with the mean field ${\it\alpha}$ coefficient zero, and is caused by the interaction between an off-diagonal component of the turbulent resistivity and the stretching of the large-scale field by shear flow. Following up on previous numerical and analytic work, this paper presents further details of the numerical evidence for the effect, as well as an heuristic description of how magnetic fluctuations can interact with shear flow to produce the required electromotive force. The pressure response of the fluid is fundamental to this mechanism, which helps explain why the magnetic effect is stronger than its kinematic cousin, and the basic idea is related to the well-known lack of turbulent resistivity quenching by magnetic fluctuations. As well as being interesting for its applications to general high Reynolds number astrophysical turbulence, where strong small-scale magnetic fluctuations are expected to be prevalent, the magnetic shear-current effect is a likely candidate for large-scale dynamo in the unstratified regions of ionized accretion disks. Evidence for this is discussed, as well as future research directions and the challenges involved with understanding details of the effect in astrophysically relevant regimes.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

Electromagnetic energy transport by tearing fluctuations in a self-organized reversed-field pinch plasma

Fluctuation measurements reveal the outward electromagnetic energy flux needed to drive the dynamo electromotive force supporting magnetic self-organization in a reversed-field pinch plasma. The radial Poynting flux due to tearing mode fluctuations is measured with an insertable probe during magnetic relaxation. This flux corresponds to transient power levels much larger than the input power and comparable to the global equilibrium magnetic energy transient loss rate. The probe measurements of this flux are roughly as predicted by a simple Poynting's theorem model upon substitution of equilibrium measurement data.

Physics↗

DOE OSTI2025

Mean-field dynamo as a quantum-like modulational instability

Presented here is a novel formulation of the mean-field dynamo as a modulational instability of magnetohydrodynamic (MHD) turbulence. This formulation, termed mean-field wave kinetics (MFWK), is based on the Weyl symbol calculus and allows describing the interaction between the mean fields (magnetic field and fluid velocity) and turbulence without requiring scale separation that is commonly assumed in the literature. The turbulence is described by the Wigner–Moyal equation for the spectrum of the two-point correlation matrix (Wigner matrix) of magnetic-field and velocity fluctuations and depicts the turbulence as an effective plasma of quantum-like particles that interact via the mean fields. Eddy–eddy interactions, which serve as ‘collisions’ in this effective plasma, are modelled within the standard minimal tau approximation to aid comparison with existing theories. Using MFWK, the non-local electromotive force is calculated for generic turbulence from first principles, modulo the limitations of MFWK. This result is then used to study, both analytically and numerically, the modulational modes of MHD turbulence, which appear as linear instabilities of the said effective quantum-like plasma of fluctuations. The standard α 2 -dynamo and other known results are reproduced as special cases. A new dynamo effect is predicted that is driven by correlations between the turbulent flow velocity and the turbulent current.

astrophysical plasmas↗

DOE OSTI2016

Enhanced spin Seebeck effect signal due to spin-momentum locked topological surface states

Spin-momentum locking in protected surface states enables efficient electrical detection of magnon decay at a magnetic-insulator/topological-insulator heterojunction. Here we demonstrate this property using the spin Seebeck effect (SSE), that is, measuring the transverse thermoelectric response to a temperature gradient across a thin film of yttrium iron garnet, an insulating ferrimagnet, and forming a heterojunction with (Bi x Sb 1–x ) 2 Te 3 , a topological insulator. The non-equilibrium magnon population established at the interface can decay in part by interactions of magnons with electrons near the Fermi energy of the topological insulator. When this decay channel is made active by tuning (Bi x Sb 1–x ) 2 Te 3 into a bulk insulator, a large electromotive force emerges in the direction perpendicular to the in-plane magnetization of yttrium iron garnet. Lastly, the enhanced, tunable SSE which occurs when the Fermi level lies in the bulk gap offers unique advantages over the usual SSE in metals and therefore opens up exciting possibilities in spintronics.

58 GEOSCIENCES↗