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At least 451 records · Page 25

Reliable Devices Yield Stable Quantum Computations

Stable quantum computation requires noisy results to remain bounded even in the presence of noise fluctuations. Yet non-stationary noise processes lead to drift in the varying characteristics of a quantum device that can greatly influence the circuit outcomes. Here we address how temporal and spatial variations in noise relate device reliability to quantum computing stability. First, our approach quantifies the differences in statistical distributions of characterization metrics collected at different times and locations using Hellinger distance. We then validate an analytical bound that relates this distance directly to the stability of a computed expectation value. Our demonstration uses numerical simulations with models informed by the washington superconducting transmon device. We find that the stability metric is consistently bounded from above by the corresponding Hellinger distance, which can be cast as a specified tolerance level. These results underscore the significance of reliable quantum computing devices and the impact for stable quantum computation.

Dasgupta, Samudra↗

Creep Property of Intermetallic Dispersive Steels for Nuclear Applications

To meet the materials performance demands of next-generation nuclear and high-temperature energy systems, a new class of intermetallic-dispersive steels (IDS) has been designed through integrated computational thermodynamics and alloy design strategies. The IDS alloys incorporate coherent L1₂ (γ′-Ni₃Al) nanoprecipitates within an Fe–Ni–Cr austenitic matrix, engineered to achieve both high temperature strength and thermodynamic stability while suppressing the formation of detrimental δ-Ni₃Nb and η-Ni₃Ti phases. Initial creep testing of Ti-IDS and TiTa-IDS alloys demonstrates rupture lives comparable to or exceeding those of Inconel 718 and ODS steels, despite being fabricated through conventional ingot metallurgy. Step-load creep tests identified a stress threshold near 300–350 MPa for the onset of tertiary creep, and in-situ neutron diffraction experiments on Ti-IDS revealed clear load partitioning between the matrix and γ′ precipitates: elastic strain is shared by both phases, while plastic strain localizes in the matrix. These results confirm that stable γ′–matrix interfaces play a dominant role in retarding dislocation motion and enhancing creep resistance. In FY26, the program will conduct repeat creep rupture testing of TiTa-IDS at 650 °C/400 MPa, initiate long-term rupture testing of TiNb-IDS, and perform TEM-based microstructural characterization to elucidate dislocation–precipitate interactions and microstructural stability. Collectively, these efforts will establish the mechanistic foundation for next-generation high-temperature structural materials based on the IDS concept.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Revisiting the role of Zr doping in Ni-rich layered cathodes for lithium-ion batteries

We report the realization of high performance Ni-rich layered cathodes remains a challenge because of the multiple degradation factors that concurrently operate during battery cycling. In particular, depletion of oxygen charge and consequent lattice oxygen instability at deep charge state accelerate the subsequent chemomechanical degradation mechanisms. Among the proposed methodologies, doping has proven to be effective in enhancing the cathode cycle life by stabilizing the layered structure. Herein, we achieved the electrochemically stabilized Ni-rich LiNi 0.92 Co 0.04 Mn 0.04 O 2 through Zr doping, resulting in a 15% increase of the capacity retention after 100 cycles. In-depth investigations are conducted to unveil the effects of Zr doping on the layered cathode, and in particular, the critical role of Zr doping on the lattice oxygen stability is systematically studied. By combining state-of-the-art magnetometer characterization, X-ray analysis, and first-principles calculation, we reveal that Zr doping positively contributes the to lattice oxygen stability by alleviating the oxygen charge loss at deep charge, thereby improving the cathode electrochemical reversibility. Our findings provide an insight into the Zr doping mechanism and help to design the Ni-rich layered oxides for future applications.

25 ENERGY STORAGE↗

Laboratory studies of lean combustion

The fundamental processes controlling lean combustion were observed for better understanding, with particular emphasis on the formation and measurement of gas-phase pollutants, the stability of the combustion process (blowout limits), methods of improving stability, and the application of probe and optical diagnostics for flow field characterization, temperature mapping, and composition measurements. The following areas of investigation are described in detail: (1) axisymmetric, opposed-reacting-jet-stabilized combustor studies; (2) stabilization through heat recirculation; (3) two dimensional combustor studies; and (4) spectroscopic methods. A departure from conventional combustor design to a premixed/prevaporized, lean combustion configuration is attractive for the control of oxides of nitrogen and smoke emissions, the promotion of uniform turbine inlet temperatures, and, possibly, the reduction of carbon monoxide and hydrocarbons at idle.

Sawyer, R. F.↗

In Situ Characterization of Interface Evolution in Argyrodite‐Based All‐Solid‐State Li Batteries

Interfacial stability is one of the critical challenges in all-solid-state Li metal batteries. Multiple processes such as solid electrolyte (SE) decomposition and lithium dendrite growth take place at the solid interfaces during cycling, leading to the overall cell failure. To deconvolute these complex processes, in situ characterization is of paramount importance to elucidate the interfacial evolution on the SE upon Li plating/stripping. Herein, an all-solid-state asymmetric in situ cell is developed that allows the direct visualization of the highly localized Li plating/stripping processes under the optical microscope. Moreover, this cell configuration enables reliable post-mortem chemical and morphological analysis of the intact SE/Li interface. Using combined scanning electron microscopy and energy-dispersive X-ray spectroscopy, the study reveals that the evolution of the Li argyrodite interface is strongly influenced by the current density, particularly in terms of chemical distribution and Li plating morphology. More specifically, the solid interface is LiCl-rich with the formation of Li cubes at low current densities, while high currents result in more uniform elemental distribution and filament morphology. These findings elucidate the dynamic evolution mechanism at solid interfaces and offer valuable guidance for developing stable solid interfaces in all-solid-state Li metal batteries.

Huang, Di↗

Final report on assessment of molten salt corrosion testing of unirradiated and ion irradiated advanced manufactured high entropy alloys

Generation IV reactors and future fusion reactor designs have led to more demanding materials performance requirements due to their increased operating temperatures, corrosive coolants, and increased radiation doses compared to the current light-water reactor fleet. Among the innovative nuclear technologies under development, molten salt reactors stand out for their potential to offer superior fuel utilization, intrinsic safety characteristics, and economic viability. Of the proposed Generation IV designs, the gas fast reactor operates at 450 to 850°C and the molten salt reactor operates at 565 to 850°C, with the molten salt reactor design needing molten salt corrosion resistant materials [1, 2]. These increased temperatures and more extreme corrosion environments necessitate higher material performance, such as creep strength, radiation-tolerant microstructures, corrosion resistance, and high-temperature tensile properties. Hastelloy-N, a nickel-based alloy with additions of molybdenum and chromium, has been successfully employed to contain molten fluoride salt at temperatures up to 705°C. However, Hastelloy-N becomes embrittled upon neutron irradiation, primarily due to the accumulation of helium produced by (n,a) transmutation reactions. Furthermore, the corrosive nature of molten fluoride and chloride salts presents a formidable challenge, as these salts can react with and dissolve alloying elements such as Cr, Mo, and Fe, leading to selective leaching, loss of protective oxide layers, and accelerated degradation. High entropy alloys (HEAs) and refractory high entropy alloys (RHEAs) have emerged as a prominent area of interest, due to their ability to achieve tailored chemical compositions for specific applications. Unlike conventional alloys, HEAs are characterized by having multiple principal elements in equimolar or near equimolar ratios, leading to an unconventional alloying strategy [3]. This alloying strategy is believed to promote unique properties, such as single-phase stabilization of chemically compatible elements, lattice distortion effects due to atomic radius differences, and proposed sluggish diffusion effects. For extreme-environment applications, RHEAs have garnered much research interest because of the possibility of creating relatively ductile materials that can operate in extremely high-temperature environments, beyond the operating temperatures where other Ni-based superalloys begin to lose strength [4-6]. Idaho National Laboratory (INL) initiated a joint international effort with the Czech Republic to explore the feasibility of manufacturing HEAs for high-temperature nuclear applications using advanced manufacturing. This effort was funded at INL by the United States Department of Energy's Office of Nuclear Energy under the Advanced Reactor Technologies and Advanced Materials and Manufacturing Technologies (AMMT) Program. The HEAs were specifically designed for the corrosive and irradiation environments experienced in gas-cooled fast reactors, molten salt reactors, and fusion power. These alloys have been manufactured by multiple processes to determine the impact of manufacturing processes on the performance of the alloys in corrosive and irradiation environments. Preliminary molten salt corrosion testing showed that equimolar MoNbTiV and MoNbTi alloys exhibit exceptional performance, with arc-melted variants demonstrating only minimal degradation after 1000 hours of exposure to molten chloride salt at 700°C. Conversely, Nb2TiVZr2 showed significant molten salt corrosion susceptibility and microstructural instability during high-temperature molten salt exposures, and was, therefore deemed unfit for molten salt reactor applications. The MoNbTiV, MoNbTi, and Nb2TiVZr2 alloys were further evaluated through ion irradiation experiments conducted at the Michigan Ion Beam Laboratory at the University of Michigan. The microstructural stability and the evolution of irradiation-induced defects were characterized to assess the irradiation resistance of each of these alloys.

36 - MATERIALS SCIENCE↗

Some Properties and Stability Results for Sector-Bounded LTI Systems

This paper presents necessary and sufficient conditions for a linear, time-invariant (LTI) system to be inside sector (n, b) in terms of linear matrix inequalities in its state-space realization matrices, which represents a generalization of similar conditions for bounded H(sub infinity)-norm systems. Further, a weaker definition of LTI systems strictly inside closed sector (a, b) is proposed, and state-space characterization of such systems is presented. Sector conditions for stability of the negative feedback interconnection of two LTI systems and for stability of LTI systems with feedback nonlinearities are investigated using the Lyapunov function approach. It is shown that the proposed weaker conditions for an LTI system to be strictly inside a sector are sufficient to establish closed-loop stability of these systems.

Gupta, Sandeep↗

Robust Stabilization of Uncertain Systems Based on Energy Dissipation Concepts

Robust stability conditions obtained through generalization of the notion of energy dissipation in physical systems are discussed in this report. Linear time-invariant (LTI) systems which dissipate energy corresponding to quadratic power functions are characterized in the time-domain and the frequency-domain, in terms of linear matrix inequalities (LMls) and algebraic Riccati equations (ARE's). A novel characterization of strictly dissipative LTI systems is introduced in this report. Sufficient conditions in terms of dissipativity and strict dissipativity are presented for (1) stability of the feedback interconnection of dissipative LTI systems, (2) stability of dissipative LTI systems with memoryless feedback nonlinearities, and (3) quadratic stability of uncertain linear systems. It is demonstrated that the framework of dissipative LTI systems investigated in this report unifies and extends small gain, passivity, and sector conditions for stability. Techniques for selecting power functions for characterization of uncertain plants and robust controller synthesis based on these stability results are introduced. A spring-mass-damper example is used to illustrate the application of these methods for robust controller synthesis.

Gupta, Sandeep↗

Structural evolution, electrochemical kinetic properties, and stability of A-site doped perovskite Sr(1-x)Yb(x)CoO(3-δ)

Mixed ionic and electronic conducting (MIEC) perovskite SrCoO(3-δ) is a widely studied (electro)catalyst for the oxygen reduction reaction (ORR) and possesses different crystal structures at different temperatures. These temperature dependent phase transitions significantly impact the ordering of oxygen vacancies and electrochemical kinetic properties as well as the reliability of the related devices. Some of the crystal structures formed, e.g. hexagonal phases, turn out to be almost impermeable to oxygen gas. Therefore, it is important to stabilize the crystal structure of SrCoO(3-δ) that favors the ORR over a wide temperature range. Herein, the partial substitution of the A-site Sr with Yb is systematically studied, including synthesis, characterization and analysis of structural evolution, electrochemical kinetic properties, thermal stability, and stability in a CO2-containing atmosphere. The results indicate that Sr(0.90)Yb(0.10)CoO(3-δ) is able to stabilize the tetragonal crystal structure with less ordered oxygen vacancies, leading to polarization resistances of 0.051, 0.115 and 0.272 U sq.cm at 750, 700 and 650 °C, respectively, on symmetrical cells. Sr(0.90)Yb(0.10)CoO(3-δ) demonstrates a very stable surface oxygen vacancy distribution and electronic structure near oxygen vacancies but dissociation of adsorbed oxygen molecules into atomic oxygen is affected by surface Sr segregation, and polarization resistance degradation is mainly induced by surface Sr segregation. Furthermore, Sr(0.90)Yb(0.10)CoO(3-δ) exhibits excellent thermal stability as well as excellent recovery stability and improved polarization performance after a few pure air/CO2-containing air treatment cycles at 700 °C. However, a hysteresis behavior of polarization performance is observed at 650 °C during gas cycling treatment, which may cause long-term degradation of the Sr(0.90)Yb(0.10)CoO(3-δ) electrode. The different polarization behaviors during gas cycling treatment are induced by different sensitivities of the formed surface strontium carbonate and chemisorbed surface oxo-carbonaceous species to different operating temperatures.

electrochemical kinetic↗

Characterization of polybenzimidazole (PBI) film at high temperatures

Polybenzimidazole, a linear thermoplastic polymer with excellent thermal stability and strength retention over a wide range of temperatures, was evaluated for its potential use as the main dielectric in high temperature capacitors. The film was characterized in terms of its dielectric properties in a frequency range of 50 Hz to 100 kilo-Hz. These properties, which include the dielectric constant and dielectric loss, were also obtained in a temperature range from 20 C to 300 C with an electrical stress of 60 Hz, 50 V/mil present. The alternating and direct current breakdown voltages of silicone oil impregnated films as a function of temperature were also determined. The results obtained indicate that while the film remained relatively stable up to 200 C, it exhibited an increase in its dielectric properties as the temperature was raised to 300 C. It was also found that conditioning of the film by heat treatment at 60 C for six hours tended to improve its dielectric and breakdown properties. The results are discussed and conclusions made concerning the suitability of the film as a high temperature capacitor dielectric.

Hammoud, Ahmad N.↗

Elucidating the role of $\mathrm{Fe}$-$\mathrm{Mo}$ interactions in the metal oxide precursors for Fe promoted $\mathrm{Mo/ZSM}$-5 catalysts in non-oxidative methane dehydroaromatization

Literature shows that adding Fe as a separate phase to MoO 3 /ZSM-5 catalysts can improve benzene selectivity in methane dehydroaromatization (MDA), but only when added in small quantities, making it difficult to characterize the state of Fe in the catalyst and understand the role of Fe-Mo interactions on the catalytic properties. We explore how the nature of the Mo-Fe interactions in the catalyst precursor can influence the stability and product selectivity in MDA, by employing for the first time Fe 2 (MoO 4 ) 3 /ZSM-5 as a catalyst precursor in MDA. We have compared the activity of Fe 2 (MoO 4 ) 3 /ZSM-5 with monometallic MoO 3 /ZSM-5 and mixed MoO 3 + Fe 2 O 3 /ZSM-5 containing equivalent Mo and Fe loadings and found that Fe 2 (MoO 4 ) 3 /ZSM-5 shows higher benzene selectivity than the mixed MoO 3 + Fe 2 O 3 /ZSM-5 catalyst and exhibits higher stability in reaction compared to the monometallic MoO3/ZSM-5 catalyst. Structural characterization suggests that Fe 2 (MoO 4 ) 3 partially segregates to Fe 2 O 3 and amorphous MoO x during thermal pretreatment. The MoO x species migrate into the zeolite channels during pretreatment, while Fe oxides remain on the external surface of the zeolite. Gas adsorption/desorption techniques and density functional theory calculations demonstrate that the preexisting Fe 2 O 3 phases on the external surface of the zeolite in the mixed MoO 3 + Fe 2 O 3 /ZSM-5 precursor trap (MoO 3 ) 3 clusters preventing them from migrating into the zeolite channels during pretreatment, whereas gradual formation of amorphous MoOx together with the segregation of the Fe 2 O 3 phase when using the Fe 2 (MoO 4 ) 3 precursor diminishes trapping of (MoO 3 ) 3 and consequently enhances migration and anchoring of the MoO x species in the zeolite channels, boosting selectivity to benzene. Characterization of used catalysts suggests that the presence of Fe promotes formation of structured carbon nanofibers which reduce the rate of catalyst deactivation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Palladium Single-Atom (In)Stability Under Aqueous Reductive Conditions

Here, we investigate the stability and performance of single-atom Pd on TiO 2 for the selective dechlorination of 4-chlorophenol. A challenge inherent to single atoms is their high surface free energy, which results in a tendency for the surface migration and aggregation of metal atoms. This work evaluates various factors affecting the stability of Pd single-atoms, including atomic dispersion, coordination environment, and substrate properties, under reductive aqueous conditions. The transition from single atoms to clusters vastly enhanced dechlorination kinetics without diminishing carbon–chlorine bond selectivity. X-ray absorption spectroscopy analysis using both in situ and ex situ conditions followed the dynamic transformation of single atoms into amorphous clusters, which consist of a unique unsaturated coordination environment and few nanometer diameter. Importantly, the intricate relationship between stability and performance underscores the vital role of detailed characterization to properly determine the true active species for dehalogenation reactions.

36 MATERIALS SCIENCE↗

Unblocking Oxygen Charge Compensation for Stabilized High‐Voltage Structure in P2‐Type Sodium‐Ion Cathode

Abstract Layered transition‐metal (TM) oxides are ideal hosts for Li + charge carriers largely due to the occurrence of oxygen charge compensation that stabilizes the layered structure at high voltage. Hence, enabling charge compensation in sodium layered oxides is a fascinating task for extending the cycle life of sodium‐ion batteries. Herein a Ti/Mg co‐doping strategy for a model P2‐Na 2/3 Ni 1/3 Mn 2/3 O 2 cathode material is put forward to activate charge compensation through highly hybridized O 2 p TM 3 d covalent bonds. In this way, the interlayer OO electrostatic repulsion is weakened upon deeply charging, which strongly affects the systematic total energy that transforms the striking P2–O2 interlayer contraction into a moderate solid‐solution‐type evolution. Accordingly, the cycling stability of the codoped cathode material is improved superiorly over the pristine sample. This study starts a perspective way of optimizing the sodium layered cathodes by rational structural design coupling electrochemical reactions, which can be extended to widespread battery researches.

25 ENERGY STORAGE↗

Changes in rock matrix compressibility during deep CO 2 storage

Geologic carbon storage projects aim to permanently trap large volumes of CO 2 in reservoir rock sealed with low permeability layers. As high-pressure supercritical or liquid CO 2 is injected, hydromechanical and chemical processes caused by the reaction between the rock and acidic mixture of brine and CO 2 are initiated. The compressibility of reservoir rock needs to be properly characterized in order to assess the deformation and stability of the host formations, and there are a number of factors to be considered, including the matrix structure, solid, pores, and fluid. Here this study triggers from a fundamental question whether CO 2 treatment affects the compressibility of the rock matrix and its dominant composing solid minerals. Three different reservoir representatives are selected: Berea sandstone for silica-rich rock, and Apulian limestone and Indiana limestone for calcite-rich rock. Quartz and calcite are the main composing minerals of the reservoir rock, and their crystals are separately examined. Experimental methods are introduced for high-pressure CO 2 treatment of water-saturated materials, and measurements of the unjacketed and solid compressibilities are conducted. No change in the solid compressibility of the sandstone and quartz after CO 2 treatment is observed, whereas it increases by 18–21% for the limestones and by 15% for calcite. The latter observation is inconsistent with the ultrasonic wave velocities measurements and is believed to be due to the local dissolution of the calcite crystal surface. Our results show that only the solid matrix of the limestones becomes more compressible after CO 2 treatment. Consequent microimaging and mercury intrusion porosimetry analyses allowed observations of dissolution and precipitation of calcite, and creation of new connected and non-connected pores. Finally, the changes in limestone solid compressibilities and pore structure could significantly affect the rock properties and behavior during and after CO 2 injection and should be accounted for in the reservoir models.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Enhanced thermal reliability and performance of calcium chloride hexahydrate phase change material using cellulose nanofibril and graphene nanoplatelet

In recent years, thermal energy storage (TES) has gained attention for its role in enhancing renewable energy solutions and sustainable energy consumption. The usage of strontium chloride hexahydrate (SCH), graphene nanoplatelet (GNP), and cellulose nanofibril (CNF) additives were investigated to enhance the performance of calcium chloride hexahydrate (CCH) based on the melting/solidification behavior for TES applications. In this work, we develop a promising phase-change-material (PCM) formulation by introducing these additives that reduce supercooling, improve the thermal conductivity and stabilizing the energy storage capacity of CCH. Rheological characterizations demonstrated that the addition of 1 wt% of CNF into CCH produced the required improvement in viscosity and boosted solid-like rheological behavior. Structural characterizations show a physical mixing of the materials within the PCM composites. Our observations show that the amphiphilicity of CNF enables the surface attachment to GNP via hydrophobic interactions providing effective dispersion of GNP throughout the PCM composite. The addition of a nucleating agent, SCH decreased the degree of supercooling of ~20 g of CCH from >20 °C to 3 °C at a cooling rate of 5 °C/min. Thermal characterization showed the resulting PCM composite has a latent heat of melting of 186 Jg -1 , phase change temperature of 32 °C, and stable thermal properties after being subjected to 70 melt-freeze cycles. Adding CNF and GNP to pure CCH increased its thermal conductivity by 76 %. The high thermal conductivity of GNP and its effective dispersion by CNF is responsible for this enhancement. The study highlights the use of biodegradable nanocellulose for the preparation of sustainable PCM composites with improved performance. In conclusion, these PCM composites are scalable, they have potential to increase energy efficiency and revolutionalize the heating/cooling applications in buildings and other TES systems.

25 ENERGY STORAGE↗

Impact of fission product inclusion on phase development in U 3 Si 2 fuel

Due to its high thermal conductivity and uranium density, U 3 S i2 has been considered as a candidate for use as an accident tolerant fuel (ATF). In order to fully assess its suitability and performance as a fuel, the impact of fission products (FPs) on the stability and performance of U 3 Si 2 must be investigated. The interactions of FPs and U 3 Si 2 have had relatively little study until now and require experimental and computational examination. U 3 Si 2 was doped with individual FPs to explore U-Si-FP interactions and phase equilibria that may impact the performance of the ATF during irradiation. Elemental Ce, Mo, Y, or Zr were used to individually dope U 3 Si 2 at a concentration of 5 wt% FP. A diffusion couple of a 1:1 Mo:Zr alloy and U 3 Si 2 was heated to 1200 °C in order to consider the impacts of multiple FPs on the stability and structure of the fuel. Samples were characterized for FP solubility and secondary phase formation using electron microscopy, energy dispersive spectroscopy, and x-ray diffraction. First principles density functional theory calculations complemented the experimental effort to understand FP behavior. Experimental and computational findings were used in the development of a thermodynamic database containing 8 major FPs and their associated silicide phases. Finally, fuel compositions generated from depletion calculations were used to thermodynamically model the equilibrium phases of the fuel undergoing burnup.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗