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DOE OSTI2016

Insight into the Catalytic Mechanism of Bimetallic Platinum–Copper Core–Shell Nanostructures for Nonaqueous Oxygen Evolution Reactions

The oxygen evolution reaction (OER) plays a critical role in multiple energy conversion and storage applications. However, its sluggish kinetics usually results in large voltage polarization and unnecessary energy loss. Therefore, designing efficient catalysts that could facilitate this process has become an emerging topic. Here, we present a unique Pt–Cu core–shell nanostructure for catalyzing the nonaqueous OER. The catalysts were systematically investigated with comprehensive spectroscopic techniques, and applied in nonaqueous Li–O2 electrochemical cells, which exhibited dramatically reduced charging overpotential (<0.2 V). The superior performance is explained by the robust Cu(I) surface sites stabilized by the Pt core in the nanostructure. The insights into the catalytic mechanism of the unique Pt–Cu core–shell nanostructure gained in this work are expected to serve as a guide for future design of other nanostructured bimetallic OER catalysts.

alloys↗

DOE OSTI2019

Low-Loss, High-Flux Saturation Magnetic Cores for Power Converters

As new and alternative energy sources are added to the energy grid, efficient and low-loss power converters are essential to the storage of energy from these intermittent power sources. Higher operating frequency can reduce the size and weight of transformers. However, current magnetic cores limit the operating frequency because core losses increase with frequency. Therefore, new magnetic core materials are needed with higher resistivity (lower eddy-current losses), lower coercivity (lower hysteresis losses), and higher permeability and flux density (higher power density). These new materials must be integrated into isolated power converters designed to optimize efficiency based on the transformer performance. To address this need, Mainstream pursued a two-pronged approach in Phase I to develop novel magnetic materials and model a planar transformer design. We irradiated silicon steel with a high-energy electron beam in an attempt to induce nanocrystalline grain formation. The nanocrystalline grains were expected to increase resistivity to reduce eddy-current losses and decrease coercivity to reduce hysteresis losses. We also modeled the transformer performance through Simulation Program with Integrated Circuit Emphasis (SPICE) and analytical models to establish the effect of magnetic properties of the core on the performance of the transformer. There still are hurdles to be overcome in Phase II. The electron beam processing was successful in increasing the resistivity and the flux saturation density. However, the resistivity is still too low for high-frequency magnetic cores, because the eddy-current losses would be prohibitively high. Additionally, the coercivity increased for the processed samples leading to higher hysteresis losses. In comparing our SPICE and analytical models to the planar transformer measured values and impedance plots, good agreement was seen for primary and secondary short-circuit impedance measurements and for primary-to-secondary capacitance measurements. The SPICE model deviated from measured values, though, when measuring the transformer open-circuit impedance, indicating that we might need to add more model complexity to the transformer model. Phase II research will continue to build on the transformer model and integrating novel magnetic materials into high-frequency transformers.

15 GEOTHERMAL ENERGY↗

DOE OSTI2017

Formation and mechanism of nanocrystalline AZ91 powders during HDDR processing

Grain sizes of AZ91 alloy powders were markedly refined to about 15 nm from 100 to 160 μm by an optimized hydrogenation-disproportionation-desorption-recombination (HDDR) process. The effect of temperature, hydrogen pressure and processing time on phase and microstructure evolution of AZ91 alloy powders during HDDR process was investigated systematically by X-ray diffraction, optical microscopy, scanning electron microscopy and transmission electron microscopy, respectively. The optimal HDDR process for preparing nanocrystalline Mg alloy powders is hydriding at temperature of 350 °C under 4 MPa hydrogen pressure for 12 h and dehydriding at 350 °C for 3 h in vacuum. A modified unreacted core model was introduced to describe the mechanism of grain refinement of during HDDR process. - Highlights: • Grain size of the AZ91 alloy powders was significantly refined from 100 μm to 15 nm. • The optimal HDDR technology for nano Mg alloy powders is obtained. • A modified unreacted core model of grain refinement mechanism was proposed.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Recursive Use of the Short-Time Fast Fourier Transform for Signature Analysis in Continuous Processes

Although a nuclear reactor is a hostile environment for sensing and electrical communications, the reactor core is amenable to acoustic communication. An acoustic measurement infrastructure (AMI) has been installed in the Advanced Test Reactor (ATR) to record acoustic signals that can capture its different operating regimes. AMI uses coolant pumps as continuous signal sources, coolant and structural components as transmission lines, and accelerometers to capture system motion. A recursive signal processing technique based on the short-time fast Fourier transform (STFFT) for continuous processes provides unique signatures for diagnostic and prognostic analyses from the system motion data. Here this article presents a recursive STFFT methodology that processes acoustic signals from continuous industrial processes. The article first discusses the initial STFFT use with simulated data to elucidate the basic principles necessary to understand and interpret the STFFT results from actual pump vibration data. Each repetitive use of the STFFT on pump vibration data using the results from the prior STFFT processing will generate additional complimentary time-frequency-based signatures. These signatures are generated by the coolant pumps operating under different process conditions. After each use of the STFFT, the resulting signatures provide exemplary examples of the diversity and intuitive nature of recursively using the STFFT. This article focuses on recursively using the STFFT to provide numerous complimentary and diverse signatures that will ultimately be inputs for machine learning algorithms that provide predictive data analytics. The intuitive nature of the information and signatures from recursive STFFT processing will also bring intuitive interpretation capabilities to machine learning and predictive data analytic techniques.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

NASA NTRS1988

The rotational dynamics of Mercury and the state of its core

Data on the rotational dynamics of Mercury are examined together with possible events that could lead to the current state of rotation. It is shown that the dynamical evolution of Mercury's spin angular momentum controlled by the dissipative processes of tidal friction and relative motion between a solid mantle and a liquid core would lead naturally to the current state of rotation of the Mercury planet. To investigate the possibility that Mercury has a molten core, an experiment is designed for the measurement of the core properties of Mercury. It is shown that it is technically feasible to measure the four parameters necessary for the determination of the existence and the extent of a Mercurian molten core, including the amplitude of the physical vibration about the resonance spin rate, the obliquity, and the gravitational harmonic coefficients.

Peale, S. J.↗

DOE OSTI2018

Pathways towards Valid Data: Assessment of Optimized Packaging Strategies for Core Components - 18158

Every company that runs nuclear power plants needs a strategy for disposal of the radioactive waste and for decommissioning and dismantling of its nuclear reactors. The dismantling progress of several German NPPs is already in an advanced stage. Hence, particularly highly activated core components have to be disposed of as radioactive waste. Nevertheless, this is also an issue during the operating phase due to necessary replacements of highly activated core components such as PWR control elements or RPV heads. The conditioning of waste packages for final disposal in the German repository Konrad requires the core components to be dismantled, packaged and dried. Therefore, a qualified packaging strategy is needed to ensure a reliable compliance with the protection objectives of the repository and an optimized utilization of prescribed contingents. Exemplified by PWR control elements a pathway is drawn how to perform an optimized packaging strategy in compliance with the protection objectives of the repository based on only few relevant radionuclides derived from activation calculations. For these calculations, particularly the influence of trace impurities in the materials has to be considered and their amounts have to be verified or analyzed by sampling. Furthermore, low nuclide activities from contamination cannot simply be neglected because some of them are obliged to be declared or their radiological relevance has not been sufficiently determined. Due to various influence factors, qualified sampling strategies need carefully considered concepts. Therefore, detailed planning facilitates the qualification and approval process and reduces the costs for analyses and the number of containers. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

Electron and ion spectroscopy of azobenzene in the valence and core shells

Azobenzene is a prototype and a building block of a class of molecules of extreme technological interest as molecular photo-switches. We present a joint experimental and theoretical study of its response to irradiation with light across the UV to x-ray spectrum. The study of valence and inner shell photo-ionization and excitation processes combined with measurement of valence photoelectron-photoion coincidence and mass spectra across the core thresholds provides a detailed insight into the site- and state-selected photo-induced processes. Photo-ionization and excitation measurements are interpreted via the multi-configurational restricted active space self-consistent field method corrected by second order perturbation theory. Using static modeling, we demonstrate that the carbon and nitrogen K edges of azobenzene are suitable candidates for exploring its photoinduced dynamics thanks to the transient signals appearing in background-free regions of the NEXAFS and XPS.

Chemistry↗

DOE OSTI2015

Synthesis, microstructure and magnetic properties of Fe{sub 3}Si{sub 0.7}Al{sub 0.3}@SiO{sub 2} core–shell particles and Fe{sub 3}Si/Al{sub 2}O{sub 3} soft magnetic composite core

Fe{sub 3}Si{sub 0.7}Al{sub 0.3}@SiO{sub 2} core–shell particles and Fe{sub 3}Si/Al{sub 2}O{sub 3} soft magnetic composite core have been synthesized via a modified stöber method combined with following high temperature sintering process. Most of conductive Fe{sub 3}Si{sub 0.7}Al{sub 0.3} particles could be uniformly coated by insulating SiO{sub 2} using the modified stöber method. The Fe{sub 3}Si{sub 0.7}Al{sub 0.3}@SiO{sub 2} core–shell particles exhibited good soft magnetic properties with low coercivity and high saturation magnetization. The reaction 4Al+3SiO{sub 2}=2α-Al{sub 2}O{sub 3}+3Si took place during the sintering process. As a result the new Fe{sub 3}Si/Al{sub 2}O{sub 3} composite was formed. The Fe{sub 3}Si/Al{sub 2}O{sub 3} composite core displayed more excellent soft magnetic properties, better frequency stability at high frequencies, much higher electrical resistivity and lower core loss than the pure Fe{sub 3}Si{sub 0.7}Al{sub 0.3} core. The method of introducing insulating layers surrounding magnetic particles provides a promising route to develop new and high compact soft magnetic materials with good magnetic and electric properties. - Graphical abstract: In Fe{sub 3}Si/Al{sub 2}O{sub 3} composite, Fe{sub 3}Si phases are separated by Al{sub 2}O{sub 3} layers and the eddy currents are confined in Fe{sub 3}Si phases, thus increasing resistivity and reducing core loss. - Highlights: • Fe{sub 3}Si{sub 0.7}Al{sub 0.3}@SiO{sub 2} core–shell particles and Fe{sub 3}Si/Al{sub 2}O{sub 3} cores were prepared. • Fe{sub 3}Si{sub 0.7}Al{sub 0.3} particles could be uniformly coated by nano-sized SiO{sub 2} clusters. • Fe{sub 3}Si{sub 0.7}Al{sub 0.3}@SiO{sub 2} particles and Fe{sub 3}Si/Al{sub 2}O{sub 3} cores showed good soft magnetic properties. • Fe{sub 3}Si/Al{sub 2}O{sub 3} had lower core loss and better frequency stability than Fe{sub 3}Si{sub 0.7}Al{sub 0.3} cores.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2016

Asymmetric unwrapping of nucleosomal DNA propagates asymmetric opening and dissociation of the histone core

The nucleosome core particle (NCP) is the basic structural unit for genome packaging in eukaryotic cells and consists of DNA wound around a core of eight histone proteins. DNA access is modulated through dynamic processes of NCP disassembly. Partly disassembled structures, such as the hexasome (containing six histones) and the tetrasome (four histones), are important for transcription regulation in vivo. However, the pathways for their formation have been difficult to characterize. We combine time-resolved (TR) small-angle X-ray scattering and TR-FRET to correlate changes in the DNA conformations with composition of the histone core during salt-induced disassembly of canonical NCPs. We find that H2A–H2B histone dimers are released sequentially, with the first dimer being released after the DNA has formed an asymmetrically unwrapped, teardrop-shape DNA structure. This finding suggests that the octasome-to-hexasome transition is guided by the asymmetric unwrapping of the DNA. Furthermore, the link between DNA structure and histone composition suggests a potential mechanism for the action of proteins that alter nucleosome configurations such as histone chaperones and chromatin remodeling complexes.

59 BASIC BIOLOGICAL SCIENCES↗

NASA NTRS1973

Trapped solar and cosmogenic noble gas abundances in Apollo 15 and 16 deep drill samples

Abundances and isotopic compositions of all the stable noble gases (He, Ne, Ar, Kr, Xe) were measured at different depths of the Apollo 15 and Apollo 16 deep drill cores, and in several surface fines and breccias. All samples analyzed from both drill cores were found to contain large concentrations of solar wind implanted gases. This means that even the deepest layers of both cores have experienced a lunar surface history. The Apollo 15 core data are consistent with a combined accretion plus static time of a few hundred million years, and also indicate variable pre-accretion irradiation of core material. Depth profiles of cosmogenic gases in the Apollo 16 core show considerably larger concentrations of cosmic gases below 65 cm depth than above. This pattern may be interpreted either as an accretionary process, or by a more recent deposition of regolith to the upper 70 cm of the core.

Bogard, D. D.↗

NASA NTRS2004

Biologically Derived Nanoparticle Arrays via a Site-Specific Reconstitution of Ferritin and their Electrochemistry

Nanoparticle arrays biologically derived from an electrochemically-controlled site-specific biomineralization were fabricated on a gold substrate through the immobilization process of biomolecules. The work reported herein includes the immobilization of ferritin with various surface modifications, the electrochemical biomineralization of ferritins with different inorganic cores, the fabrication of self-assembled arrays with the immobilized ferritin, and the electrochemical characterization of various core materials. Protein immobilization on the substrate is achieved by anchoring ferritins with dithiobis-N-succinimidyl propionate (DTSP). A reconstitution process of electrochemical site-specific biomineralization with a protein cage loads ferritins with different core materials such as Pt, Co, Mn, and Ni. The ferritin acts as a nano-scale template, a biocompatible cage, and a separator between the nanoparticles. The nano-sized metalcored ferritins on a gold substrate displayed a good electrochemical activity for the electron transport and storage, which is suitable for bioelectronics applications such as biofuel cell, bionanobattery, biosensors, etc. Keywords: Ferritin, immobilization, site-specific reconstitution, biomineralization, and bioelectronics

Kim, Jae-Woo↗

DOE OSTI2020

P SI4 1.4: Open-source software for high-throughput quantum chemistry

PSI4 is a free and open-source ab initio electronic structure program providing implementations of Hartree–Fock, density functional theory, many-body perturbation theory, configuration interaction, density cumulant theory, symmetry-adapted perturbation theory, and coupled-cluster theory. Most of the methods are quite efficient, thanks to density fitting and multi-core parallelism. The program is a hybrid of C++ and Python, and calculations may be run with very simple text files or using the Python API, facilitating post-processing and complex workflows; method developers also have access to most of PSI4 's core functionalities via Python. Job specification may be passed using The Molecular Sciences Software Institute (MolSSI) QCSCHEMA data format, facilitating interoperability. We announce a rewrite of our top-level computation driver, and concomitant adoption of the MolSSI QCARCHIVE INFRASTRUCTURE project, makes the latest version of PSI4 well suited to distributed computation of large numbers of independent tasks. The project has fostered the development of independent software components that may be reused in other quantum chemistry programs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1992

Space Station Furnace Facility Core. Requirements definition and conceptual design study. Volume 2: Technical report. Appendix 6: Technical summary reports

The Space Station Furnace Facility (SSFF) is a modular facility for materials research in the microgravity environment of the Space Station Freedom (SSF). The SSFF is designed for crystal growth and solidification research in the fields of electronic and photonic materials, metals and alloys, and glasses and ceramics and will allow for experimental determination of the role of gravitational forces in the solidification process. The facility will provide a capability for basic scientific research and will evaluate the commercial viability of low-gravity processing of selected technologically important materials. The facility is designed to support a complement of furnace modules as outlined in the Science Capabilities Requirements Document (SCRD). The SSFF is a three rack facility that provides the functions, interfaces, and equipment necessary for the processing of the furnaces and consists of two main parts: the SSFF Core Rack and the two Experiment Racks. The facility is designed to accommodate two experimenter-provided furnace modules housed within the two experiment racks, and is designed to operate these two furnace modules simultaneously. The SCRD specifies a wide range of furnace requirements and serves as the basis for the SSFF conceptual design. SSFF will support automated processing during the man-tended operations and is also designed for crew interface during the permanently manned configuration. The facility is modular in design and facilitates changes as required, so the SSFF is adept to modifications, maintenance, reconfiguration, and technology evolution.

Source record↗

DOE OSTI2025

Novel Synthesis and Characterization of Uranium-Zirconium Carbonitride by Direct Casting

UZrCN has exhibited thermophysical properties beneficial to high temperature reactor applications such as nuclear thermal rockets. The present work investigates a novel liquid phase synthesis method involving the admission of nitrogen gas during arc melting of uranium, zirconium, and carbon. Initial microstructural examinations using SEM indicated that the samples remain heterogenous with zirconium-rich cores in a uranium-rich matrix. Heterogeneity resulted from large differences in melting temperature of the major constituents and rapid solidification. Additional EDS, combustion analysis, and inert gas fusion analysis proved that the core regions have both uranium and zirconium and establish that carbon and nitrogen are retained during the fabrication process. XRD clarifies that the light elements did not form compounds with the uranium matrix but rather incorporated into the core region forming a sub-stoichiometric UZrCN. Heat treatment performed on equimolar U-Zr-C resulted in an increase in the homogenous phase present with an XRD pattern reflecting a ternary UZrCN despite small amounts of segregation in the final button.

36 - MATERIALS SCIENCE↗

DOE OSTI2025

On Uranium-Zirconium Carbonitride Formation by Direct Casting - A Novel Synthesis Study

36 - MATERIALS SCIENCE↗

DOE OSTI2016

CHEMICAL AND PHYSICAL CHARACTERIZATION OF COLLAPSING LOW-MASS PRESTELLAR DENSE CORES

The first hydrostatic core, also called the first Larson core, is one of the first steps in low-mass star formation as predicted by theory. With recent and future high-performance telescopes, the details of these first phases are becoming accessible, and observations may confirm theory and even present new challenges for theoreticians. In this context, from a theoretical point of view, we study the chemical and physical evolution of the collapse of prestellar cores until the formation of the first Larson core, in order to better characterize this early phase in the star formation process. We couple a state-of-the-art hydrodynamical model with full gas-grain chemistry, using different assumptions for the magnetic field strength and orientation. We extract the different components of each collapsing core (i.e., the central core, the outflow, the disk, the pseudodisk, and the envelope) to highlight their specific physical and chemical characteristics. Each component often presents a specific physical history, as well as a specific chemical evolution. From some species, the components can clearly be differentiated. The different core models can also be chemically differentiated. Our simulation suggests that some chemical species act as tracers of the different components of a collapsing prestellar dense core, and as tracers of the magnetic field characteristics of the core. From this result, we pinpoint promising key chemical species to be observed.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2019

BigPanDA: PanDA Workload Management System and its Applications beyond ATLAS

Modern experiments collect peta-scale volumes of data and utilize vast, geographically distributed computing infrastructure that serves thousands of scientists around the world. Requirements for rapid, near real-time data processing, fast analysis cycles and need to run massive detector simulations to support data analysis pose special premium on efficient use of available computational resources. A sophisticated Workload Management System (WMS) is needed to coordinate the distribution and processing of data and jobs in such environment. The ATLAS experiment at CERN uses PanDA (Production and Data Analysis) Workload Management System for managing the workflow for all data processing on over 150 data centers. While PanDAcurrently uses more than 250,000 cores with a peak performance of 0.3 petaFLOPS, it runs around 2 million jobs per day on hundreds of Grid sites and serving thousands of ATLAS users. In 2017 about 1.5 exabytes of data were processed with PanDA.In 2012 BigPanDA project project was started with aim to introduce new types of computing resources into ATLAS computing infrastructure, but also to offering PanDA features to different data-intensive applications for projects and experiments outside of ATLAS and High-Energy and Nuclear Physics. In this article we will present accomplishments and discuss possible directions for future work.

Svirin, Pavlo↗

DOE OSTI2020

Solid-State Sintering of Core-Shell Ceramic Powders Fabricated by Particle Atomic Layer Deposition

The properties of technical ceramics are highly dependent on their microstructure, which evolves during sintering. Sintering is the process by which ceramic parts are subjected to high temperatures to activate chemical diffusion and the consumption of porosity. During the initial stage of sintering, interparticle necks between neighboring particles form and subsequently increase in size, consuming porosity as the particle centers move closer together. To experimentally determine how this process depends on particle surface composition, particle atomic layer deposition (ALD) was used to deposit a thin film of amorphous aluminum oxide (Al2O3) onto yttria-stabilized tetragonal zirconia (3YSZ) particles, producing core-shell structured powders. The uniformity of the Al2O3 film was confirmed with transmission electron microscopy and energy dispersive spectroscopy. Scanning electron microscopy was used to observe microstructural evolution during sintering, and the dihedral angles of Al2O3 and 3YSZ grains were measured to determine the ratio of interfacial energies between the 3YSZ|3YSZ, 3YSZ|Al2O3, and Al2O3|Al2O3 interfaces. Analysis of the densification kinetics revealed that the initial stage of densification is dependent on the material at the surface of the particles (ie, the Al2O3 film) and is controlled by the diffusion of Al3+ cations through Al2O3. Once the Al2O3 film has coalesced, the sintering behavior is controlled by the densification of the core material (3YSZ). Thus, core-shell powders fabricated by particle ALD sinter by a two-step process where the kinetics are dependent on the material present at interparticle contacts.

alumina↗