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618 records · Page 35
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Engineering Nanostructured Interfaces of Hexagonal Boron Nitride-Based Materials for Enhanced Catalysis

Hexagonal boron nitrides (h-BNs) are attractive two-dimensional (2D) nanomaterials that consist of alternating B and N atoms and layered honeycomb-like structures similar to graphene. They have exhibited unique properties and promising application potentials in the field of energy storage and transformation. Recent advances in utilizing h-BN as a metal-free catalyst in the oxidative dehydrogenation of propane have triggered broad interests in exploring h-BN in catalysis. However, h-BN-based materials as robust nanocatalysts in heterogeneous catalysis are still underexplored because of the limited methodologies capable of affording h-BN with controllable crystallinity, abundant porosity, high purity, and defect engineering, which played important roles in tuning their catalytic performance. Here, in this account, our recent progress in addressing the above issues will be highlighted, including the synthesis of high-quality h-BN-based nanomaterials via both bottom-up and top-down pathways and their catalytic utilization as metal-free catalysts or as supports to tune the interfacial electronic properties on the metal nanoparticles (NPs). First, we will focus on the large-scale fabrication of h-BN nanosheets (h-BNNSs) with high crystallinity, improved surface area, satisfactory purity, and tunable defects. h-BN derived from the traditional approaches using boron trioxide and urea as the starting materials generally contains carbon/oxygen impurities and has low crystallinity. Several new strategies were developed to address the issues. Using bulk h-BN as the precursor via gas exfoliation in liquid nitrogen, single- or few-layered h-BNNS with abundant defects could be generated. Amorphous h-BN precursors could be converted to h-BN nanosheets with high crystallinity assisted by a magnesium metallic flux via a successive dissolution/precipitation/crystallization procedure. The as-fabricated h-BNNS featured high crystallinity and purity as well as abundant porosity. An ionothermal metathesis procedure was developed using inorganic molten salts (NaNH 2 and NaBH 4 ) as the precursors. The h-BN scaffolds could be produced on a large scale with high yield, and the as-afforded materials possessed high purity and crystallinity. Second, utilization of the as-prepared h-BN library as metal-free catalysts in dehydrogenation and hydrogenation reactions will be summarized, in which they exhibited enhanced catalytic activity over the counterparts from the previous synthesis method. Third, the interface modulation between metal NPs with the as-prepared defects’ abundant h-BN support will be highlighted. The h-BN-based strong metal–support interaction (SMSI) nanocatalysts were constructed without involving reducible metal oxides via the ionothermal procedure we developed by deploying specific inorganic metal salts, acting as robust nanocatalysts in CO oxidation. Under conditions simulated for practical exhaust systems, promising catalytic efficiency together with high thermal stability and sintering resistance was achieved. Across all of these examples, unique insights into structures, defects, and interfaces that emerge from in-depth characterization through microscopy, spectroscopy, and diffraction will be highlighted.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Real-time signal detection for Cyclotron Radiation Emission Spectroscopy measurements using antenna arrays

Cyclotron Radiation Emission Spectroscopy (CRES) is a technique for precision measurement of the energies of charged particles, which is being developed by the Project 8 Collaboration to measure the neutrino mass using tritium beta-decay spectroscopy. Project 8 seeks to use the CRES technique to measure the neutrino mass with a sensitivity of 40 meV, requiring a large supply of tritium atoms stored in a multi-cubic meter detector volume. Antenna arrays are one potential technology compatible with an experiment of this scale, but the capability of an antenna-based CRES experiment to measure the neutrino mass depends on the efficiency of the signal detection algorithms. Here, in this paper, we develop efficiency models for three signal detection algorithms and compare them using simulations from a prototype antenna-based CRES experiment as a case-study. The algorithms include a power threshold, a matched filter template bank, and a neural network based machine learning approach, which are analyzed in terms of their average detection efficiency and relative computational cost. It is found that significant improvements in detection efficiency and, therefore, neutrino mass sensitivity are achievable, with only a moderate increase in computation cost, by utilizing either the matched filter or machine learning approach in place of a power threshold, which is the baseline signal detection algorithm used in previous CRES experiments by Project 8.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2024

Watching a signaling protein function: What has been learned over four decades of time-resolved studies of photoactive yellow protein

Photoactive yellow protein (PYP) is a signaling protein whose internal p-coumaric acid chromophore undergoes reversible, light-induced trans-to-cis isomerization, which triggers a sequence of structural changes that ultimately lead to a signaling state. Since its discovery nearly 40 years ago, PYP has attracted much interest and has become one of the most extensively studied proteins found in nature. The method of time-resolved crystallography, pioneered by Keith Moffat, has successfully characterized intermediates in the PYP photocycle at near atomic resolution over 12 decades of time down to the sub-picosecond time scale, allowing one to stitch together a movie and literally watch a protein as it functions. But how close to reality is this movie? To address this question, results from numerous complementary time-resolved techniques including x-ray crystallography, x-ray scattering, and spectroscopy are discussed. Emerging from spectroscopic studies is a general consensus that three time constants are required to model the excited state relaxation, with a highly strained ground-state cis intermediate formed in less than 2.4 ps. Persistent strain drives the sequence of structural transitions that ultimately produce the signaling state. Crystal packing forces produce a restoring force that slows somewhat the rates of interconversion between the intermediates. Moreover, the solvent composition surrounding PYP can influence the number and structures of intermediates as well as the rates at which they interconvert. When chloride is present, the PYP photocycle in a crystal closely tracks that in solution, which suggests the epic movie of the PYP photocycle is indeed based in reality.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2004

Design of Timer Circuit for Dynamic Data System

The Branch That I work in is in the Aero Electronic Test Branch, which is part of the Research and Testing Division. The Aero Electronic Test Branch deals with electronic control and instrumentation systems. This branch supports the research and test study of wind tunnels such as the l0x10,9x15, and 8x6. Wind tunnels are used in research to test certain parts of a jet, plane, shuttle or any other flying object in certain test conditions. My assignment is to design a programmable trigger circuit on a 19 standard rack mount that will allow the circuit to latch and hold for a predefined amount of time entered by the user when receiving a signal. It should then re-arm itself within 0.25 seconds after the time is finished. The time should be able to be seen on a display showing the time entered. The time range has to be from 0-600 seconds in 0.01 second increments (600.00). From the information given, counters will be needed to design and build this circuit. A counter, in it s simplest form, is a group of flip flops that can temporarily store bits of information put into the circuit. They can be constructed in many different ways, such as in 4 flip flops (4-bit counter) or 8 flip flops and even higher. Counters are usually cascaded with other counters to reach higher bits, such as 16 or 24 bit counters. The application in which I will use the counters will be to count down from any programmable number that I input either by a keyboard or a thumbwheel. Also, I will use counters that will be used specifically as a frequency divider to divide the pulses that enter the circuit through an input signal from a crystal clock. The pulses will need to be divided so that it will function as a 100Hz clock putting out 100 pulses per second. A switch will be used to load my inputs in and more than likely a button also so that I can stop and hold the count at any point of time. I will use 5 BCD up/down programmable counters, and a certain amount (depending on what kind of "divide by N" counter I use) of frequency dividing counters for the assignment. After the design is carefully made, a task order will be written and then given to the manufacturer to create a rack mount circuit board that will match my specifications given. The applications in which this design will be used for is in the use of the six-component balance signal conditioner for measurement and electronic system control. It can be used as a timer system for the balance signal conditioner in which it does numerous tests for the Wind tunnel research, in which a preset time can be set for how long it performs its tests. Specifically, my design should be applied to the balance signal conditioner used for the 8x6 wind tunnel research. Hopefully this design should aid in more efficient research for the 8x6 wind tunnel.

Young, Nathaniel, III↗
DOE OSTI2024

From Coherence to Function: Exploring the Connection in Chemical Systems

The role of quantum mechanical coherences or coherent superposition states in excited state processes has received considerable attention in the last two decades largely due to advancements in ultrafast laser spectroscopy. These coherence effects hold promise for enhancing the efficiency and robustness of functionally relevant processes, even when confronted with energy disorder and environmental fluctuations. Understanding coherence deeply drives us to unravel mechanisms and dynamics controlled by order and synchronization at a quantum mechanical level, envisioning optical control of coherence to enhance functions or create new ones in molecular and material systems. In this frontier, the interplay between electronic and vibrational dynamics, specifically the influence of vibrations in directing electronic dynamics, has emerged as the leading principle. Here, two energetically disparate quantum degrees of freedom work in-sync to dictate the trajectory of an excited state reaction. Moreover, with the vibrational degree being directly related to the structural composition of molecular or material systems, new molecular designs could be inspired by tailoring certain structural elements. In the realm of chemical kinetics, our understanding of the dynamics of chemical transformations is underpinned by fundamental theories, such as transition state theory, activated rate theory, and Marcus theory. These theories elucidate reaction rates by considering the energy barriers that must be overcome for reactants to transform into products. Those barriers are surmounted by the stochastic nature of energy gap fluctuations within reacting systems, emphasizing that the reaction coordinate, the pathway from reactants to products, is not rigidly defined by a specific vibrational motion but encompasses a diverse array of molecular motions. While less is known about the involvement of specific intramolecular vibrational modes, their significance in certain cases cannot be overlooked. In this Account, we summarize key experimental findings that offer deeper insights into the complex electronic–vibrational trajectories encompassing excited states afforded from state-of-the-art ultrafast laser spectroscopy in three exemplary processes: photoinduced electron transfer, singlet–triplet intersystem crossing, and intramolecular vibrational energy flow in molecular systems. We delve into the rapid decoherence, or loss of phase and amplitude correlations, of vibrational coherences along promoter vibrations during subpicosecond intersystem crossing dynamics in a series of binuclear platinum complexes. This rapid decoherence illustrates the vibration-driven reactive pathways from the Franck–Condon state to the curve crossing region. We also explore the generation of new vibrational coherences induced by impulsive reaction dynamics rather than by the laser pulse in these systems, which sheds light on specific energy dissipation pathways and thereby on the progression of the reaction trajectory in the vicinity of the curve crossing on the product side. Another property of vibrational coherences, amplitude, reveals how energy can flow from one vibration to another in the electronic excited state of a terpyridine–molybdenum complex hosting a nonreactive dinitrogen substrate. In conclusion, a slight change in vibrational energy triggers a quasi-resonant interaction, leading to constructive wavepacket interference and ultimately intramolecular vibrational redistribution from a Franck–Condon active terpyridine vibration to a dinitrogen stretching vibration, energizing the dinitrogen bond.

Electrical energy↗
DOE OSTI2018

Materials for Advanced Ultra-Supercritical (AUSC) Steam Turbines – AUSC Component Demonstration

The work by the United States Department of Energy (U.S. DOE)/Ohio Coal Development Office (OCDO) Advanced Ultra-Supercritical (AUSC) Steam Boiler and Turbine Materials Consortia from 2001 through September 2015 was primarily focused on lab scale and pilot scale materials testing. The field testing included air-cooled probes and steam-cooled “loops” that were installed into existing utility boilers to gain exposure of these materials to realistic conditions of high temperature and corrosion due to the constituents in the coal ash. Successful research and development resulted in identification of metallic alloy materials and fabrication processes suited for power generation applications with metal temperatures up to approximately 1472°F (800°C). These materials or alloys have shown, in extensive laboratory tests and shop fabrication studies, to have excellent applicability for high-efficiency low CO2 transformational power generation technologies. However, as valuable as these material field tests have been for obtaining information, their scale is significantly below that required to minimize the risk associated with a power company building a multi-billion-dollar AUSC power plant. To decrease the identified risk barriers to full-scale implementation of these advanced materials, the U.S. DOE/OCDO AUSC Steam Boiler and Turbine Materials Consortia identified the key areas of the technology that need to be tested at a larger scale. Based upon the recommendations and outcome of a Consortia-sponsored workshop with the U.S.’s leading utilities, a Component Test (ComTest) Program for AUSC was proposed. The AUSC ComTest program would define materials performance requirements, plan for overall advanced system integration, design critical component tests, fabricate components for testing from advanced materials, and carry out the tests. A Pre-FEED evaluation of the test facility including the evaluation of three potential sites has been completed and previously reported. This report describes the Front-End Engineering Design (FEED), Detailed Engineering and the Environmental Assessment of the ComTest project. A significant amount of work was accomplished during Phase 1 to identity the components, as well as the component size, that would be manufactured from advanced alloys such as INCONEL 740H or HAYNES 282 alloys. Pathways to supply these components for ComTest have been identified as well as any further development that would be required. Every project of this nature has challenges and this project was no exception. The greatest challenge has been the project cost. Largely due to the infrastructure and balance of plant equipment upgrades required for Youngstown Thermal, the estimated project cost for the “base case” project was greater than originally budgeted. The project team spent a significant amount of time exploring opportunities for reducing the project cost. These options included: • Youngstown Thermal was exploring building a Combined Heat and Power (CHP) unit at their facility. The Youngstown Thermal staff, supported by Thermal Engineering Group, worked with the project team to determine whether it was economically desirable to supply ComTest with steam and other utilities, which would be supplied by the CHP project. • The project team also evaluated opportunities to optimize the project scope to reduce cost, such as reducing project scope by eliminating the Superheater Outlet Header test. • Southern Company had offered two sites as possible host locations for ComTest. Both sites had infrastructure in place such as steam from an existing unit, natural gas, cooling water and ample electrical power that would be required to be added at the Youngstown Thermal site. Utilizing this existing infrastructure could reduce the project cost. An additional project challenge was the departure of Babcock and Wilcox from the project in September 2016. This project setback was overcome by GE Power’s willingness to assume the design of the ComTest superheater. Since the project could not proceed without the superheater, this was a very positive project development. The merger of the GE Power and Alstom Power steam turbine divisions created synergies leading to the conclusion that instead of building a small-scale turbine, a more practical and useful endeavor would be to validate the manufacturing technology and supplier readiness for fabricating and machining full scale steam turbine components. Consequently, in March 2017, GE Power decided that a steam turbine test would not be necessary as part of the ComTest demonstration. Removing the operational testing of the steam turbine from ComTest further reduced the total project cost. Additionally, there was an opportunity to move ComTest from Youngstown Thermal to one of the Southern Company sites and operate ComTest at supercritical steam conditions and test the steam turbine main stop/control valve at a temperature and pressure that would be representative of the conditions of a high pressure steam turbine inlet valve. The steam could also possibly be returned to the host boiler so there would be no economic penalty of using this steam for ComTest. Relocating the project could further reduce the project cost due to the infrastructure already in place, including high pressure natural gas and cooling water, and the potential for heat integration, allowing a reduction of operating costs. Due to these potential cost reductions, it was decided to move the project away from Youngstown Thermal in March 2017. As integrating ComTest at the Southern Company site was explored, an issue was raised regarding the integration of the ComTest cycle with the plant steam cycle. Steam would be supplied to ComTest at nominally ~3865 psia and 775°F. The steam would be heated with natural gas to 1400°F for the valve test and then cooled to 1000°F so that the steam would be returned to the host boiler at the same conditions as their high pressure steam turbine inlet. However, there were concerns raised that the addition of the energy (natural gas) to the steam could trigger a New Source Review on the unit. Southern Company did not want ComTest to cause this review, so condensing all of the steam exiting ComTest and returning it to the host steam cycle as condensate was explored to insure there would be no implication that ComTest was adding energy to the host plant’s steam cycle. Ultimately, Southern Company decided that they wanted to “decouple” ComTest from the operating unit, making ComTest self-supporting, similar to the Youngstown Thermal “base case.” Without the steam turbine, the project team reached a consensus that operating the ComTest Superheater and steam turbine valves at the typical pressure of a package boiler (~1000 psig) would not generate enough useful technical information to justify the cost of the test. Therefore, it was decided in the December 2017 project quarterly meeting to cancel the operational phase of ComTest. Throughout the engineering phase of ComTest, manufacturing and supply chain challenges were identified. When GE Power recommended dropping the steam turbine test from ComTest, they identified many important manufacturing issues that should be evaluated and demonstrated. Other challenges had been raised by the GE Power group designing the superheater as well as those engineering components such as pressure relief and steam turbine bypass valves. In the December 2017 meeting, the project team decided that it was more beneficial to the AUSC technology to pursue these manufacturing and supply chain issues as Phase 2 of the ComTest project. This report is organized in the following manner: • Section 2 discusses the ComTest project background and organization. • Section 3 discussed project management. • Section 4 discusses the design of the ComTest AUSC components – the Superheater, steam turbine and Superheater Outlet Header. • Section 5 discusses the implementation of ComTest at Youngstown Thermal and the Southern Company site. • Section 6 discusses the development of the AUSC Supply Chain • Section 7 discusses the recommended plan for Phase 2 of ComTest

01 COAL, LIGNITE, AND PEAT↗