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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 739 records · Page 41

Light-driven hydrogen evolution via a novel pincer/no pincer mechanism including a possible concerted proton electron transfer

The road to efficient molecular catalysts for artificial photosynthesis requires a great deal of basic research to address the challenges of anthropogenic global warming. An unexpected result of such research is a novel pincer/no pincer mechanism discovered for the DFT-calculated catalytic cycle of PNP-C2 complexes. Structural parameters from theoretical modeling are supported by single crystal X-ray data for the corresponding complexes. Using the examples of [M(II)Cl(PNP-C2-R)] + (M = Pd 2+ , Ni 2+ ; R = CH 3 , H; PNP-C2 = N,N-bis{(di(2-methoxy-phenyl)phosphanyl)ethyl}-N-alkylamine) this pincer/no pincer mechanism is supported by differential pulse voltammetric, cyclic voltammetric, UV-Vis spectroscopic (combined with voltammetry) and 31 P nuclear magnetic resonance spectroscopic studies. The efficiency of hydrogen evolution during artificial photosynthesis depends significantly on the ratio of photosensitiser and water reduction catalysts. At first sight, the results from irradiation experiments (gas chromatography and mass spectrometry) seem obvious, but show a considerable impact of secondary and tertiary amines within the pincer structure. The best result obtained for the palladium pincer complex was with a secondary amine as a proton relay, delivering a turnover number of 2237 after only 2.5 hours. In contrast the analogous water reduction catalyst with a methylated (tertiary) amine instead of a secondary one gives only 972 turnovers under the same experimental conditions, over the same time. For all photocatalytic measurements the amount of hydrogen is approximately 2.5-times higher when a secondary amine is used as the proton relay. The influences of these different amines on the activity of water reduction catalysts during irradiation experiments in H 2 O or D 2 O lead to evidence of a kinetic isotope effect, supporting a possible concerted proton electron transfer. DFT calculations of reaction enthalpies, activation energies and intrinsic reaction coordinates of the catalytic cycle support the high efficiency of the presented catalysts. In particular, results from secondary amines suggest new candidates as examples of the rarely known concerted proton electron transfer.

14 SOLAR ENERGY↗

Kinetic simulation of a 50 mTorr capacitively coupled argon discharge over a range of frequencies and comparison to experiments

The effect of driving frequency in the range of 13.56–73 MHz on electron energy distribution and electron heating modes in a 50 mTorr capacitively coupled argon plasma discharge is studied using 1D-3V particle-in-cell simulations. Calculated electron energy probability functions exhibit three distinct “temperatures” for low-, mid-, and high-energy electrons at all the studied driving frequencies. When compared to published experimental data, the calculated probability functions show a reasonable agreement for the energy range resolved in the measurements (about 2–10 eV). Discrepancies due to limitations in experimental energy resolution outside this range lead to differences between computational and experimental values of the electron number density determined from the distribution functions, and the predicted effective electron temperature is within 25% of experimental values. The impedance of the discharge is interpreted in terms of a homogeneous equivalent circuit model, and the driving frequency dependence of the inferred combined sheath thickness is found to obey a known, theoretically derived, power law. The average power transferred from the field to the electrons (electron heating) is computed, and a region of negative heating near the sheath edge, particularly at higher driving frequencies, is identified. Analysis of the electron momentum equation shows that electron inertia, which on temporal averaging would be zero in a linear regime, is responsible for negative values of power deposition near the sheath edge at high driving frequencies due to the highly nonlinear behavior of the discharge.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Phase-space entropy cascade and irreversibility of stochastic heating in nearly collisionless plasma turbulence

We consider a nearly collisionless plasma consisting of a species of “test particles” in one spatial and one velocity dimension, stirred by an externally imposed stochastic electric field—a kinetic analog of the Kraichnan model of passive advection. The mean effect on the particle distribution function is turbulent diffusion in velocity space—known as stochastic heating. Accompanying this heating is the generation of fine-scale structure in the distribution function, which we characterize with the collisionless (Casimir) invariant C 2 ∝ ∫ ∫ d x d v 〈 f 2 〉 —a quantity that here plays the role of (negative) entropy of the distribution function. We find that C 2 is transferred from large scales to small scales in both position and velocity space via a phase-space cascade enabled by both particle streaming and nonlinear interactions between particles and the stochastic electric field. We compute the steady-state fluxes and spectrum of C 2 in Fourier space, with k and s denoting spatial and velocity wave numbers, respectively. In our model, the nonlinearity in the evolution equation for the spectrum turns into a fractional Laplacian operator in k space, leading to anomalous diffusion. Whereas even the linear phase mixing alone would lead to a constant flux of C 2 to high s (towards the collisional dissipation range) at every k , the nonlinearity accelerates this cascade by intertwining velocity and position space so that the flux of C 2 is to both high k and high s simultaneously. Integrating over velocity (spatial) wave numbers, the k -space ( s -space) flux of C 2 is constant down to a dissipation length (velocity) scale that tends to zero as the collision frequency does, even though the rate of collisional dissipation remains finite. The resulting spectrum in the inertial range is a self-similar function in the ( k , s ) plane, with power-law asymptotics at large k and s . Our model is fully analytically solvable, but the asymptotic scalings of the spectrum can also be found via a simple phenomenological theory whose key assumption is that the cascade is governed by a “critical balance” in phase space between the linear and nonlinear timescales. We argue that stochastic heating is made irreversible by this entropy cascade and that, while collisional dissipation accessed via phase mixing occurs only at small spatial scales rather than at every scale as it would in a linear system, the cascade makes phase mixing even more effective overall in the nonlinear regime than in the linear one. Published by the American Physical Society 2024

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Development of High-QE GaN Photodectors for Liquid Noble Particle Detectors

Detection of the handful of photons generated when a dark matter particle interacts in a liquid Xenon detector requires a new type of photodetector with very high detection efficiency at ultraviolet wavelengths, very low radioactive backgrounds, and essentially no measureable readout noise (achieved with devices with high intrisic gain). Such devices would find wide applicability to not only high energy physics experiments, but to a number of commercial applications including, e.g., biomedical imaging of fluorescent tags. We developed photodetectors based on amorphous GaN thin film structures (photocathodes) grown by molecular beam epitaxy on quartz windows. We also developed approaches to integrate these photocathode device structures with vacuum electron multipliers. All materials and fabrication techniques were developed to minimize radioactive backgrounds in materials, so these detectors could be used for very low count rate experiments, such as the future liquid-Xenon dark matter detectors, and future liquid-Argon neutrino detectors. We demonstrated growth of very high quantum efficiency amorphous GaN cathodes grown on a number of different substrates (Stainless steel, p-Silicon) reaching detection efficiencies of 80% at 220nm. The key to this growth was to use nitrogen plasma-assistend MBEs and very low growth temperatures. We also discovered that thinner structures (e.g.,40nm a-GaN thin films) had the best performance. We successfully demonstrated techniques for the vacuum transfer of these photocathode structures to a novel chamber that used hydraulics and bellow to form a cold indium bond needed to integrate these cathodes into sealed-tube devices. A complete, stand-along, device could not be completed during this proposal period due to difficulties in growing structures on the thick quartz window. Subsequent work is aimed at addressing this difficulty, by growing a buffer layer on the quartz substrate.

07 ISOTOPE AND RADIATION SOURCES↗

Increasing the Usability of Sockeye: Implementing Customer-Driven Modeling Improvements, Features, and Documentation of Sockeye

A number of tasks for the heat pipe simulation tool Sockeye were identified based on customer needs and included both user documentation and code development: (a) Implement saturation-dependence in the capillary pressure model; (b) Provide an analytic utility to analyze the frozen startup limit; (c) Demonstrate custom friction closures; (d) Develop examples for different types of heat transfer sources and boundary conditions; (e) Demonstrate the capillary and sonic limits; and (f) Provide discretization details in the theory manual. These tasks were all completed, and results are given where applicable.

97 MATHEMATICS AND COMPUTING↗

Bayesian Estimation of Oscillator Parameters: Toward Anomaly Detection and Cyber-Physical System Security

Cyber-physical system security presents unique challenges to conventional measurement science and technology. Anomaly detection in software-assisted physical systems, such as those employed in additive manufacturing or in DNA synthesis, is often hampered by the limited available parameter space of the underlying mechanism that is transducing the anomaly. As a result, the formulation of anomaly detection for such systems often leads to inverse or ill-posed problems, requiring statistical treatments. Here, we present Bayesian inference of unknown parameters associated with a generic actuator considered as a representative vital element of a cyber-physical system. Via a series of experimental input-output measurements, a transfer function for the actuator is obtained numerically, which serves as our model for the proposed method. Linear, nonlinear, and delayed dynamics may be assumed for the actuator response. By devising a code-based malicious signal, we study the efficacy of Bayesian inference for its potential to produce a detection, including uncertainty quantification, with a remarkably small number of input data points. Our approach should be adaptable to a variety of real-time cyber-physical anomaly detection scenarios.

47 OTHER INSTRUMENTATION↗

Photolithography system including selective light array

A system, device, and method for imparting or transferring a geometric pattern on the surface of a substrate. The device comprises, a housing forming at least a partially enclosed space, a light source body comprising an array of light emitters, a base disposed below the light source body and configured for supporting the substrate having a photoresist layer thereon, and a controller for activating a predetermined number of individual light emitters corresponding to the predetermined geometric pattern. Each individual light emitter within the array of light emitters is selectively activatable to emit a light. The array of light emitters comprises a plurality of light-emitting diodes, a plurality of quantum dots, or both.

Young, Barbara Diane↗

Revolutionizing Turbine Cooling with Micro-Architectures Enabled by Direct Metal Laser Sintering

The objective of this research effort was to explore innovative cooling architectures enabled by additive manufacturing techniques for improved turbine cooling performance. The ability to create complex internal geometries was leveraged to better distribute coolant as well as to integrate inherently unstable flow devices to enhance internal and external heat transfer. This was accomplished with a multi-faceted approach including analytical, experimental, and computational components. This final report documents progress during the total 4.25 year effort that was extended (at no additional cost) from the original 3-year cooperative agreement. Prior to starting the project, significant effort was invested in investigating innovative cooling designs from the open literature. When the project started, we quickly down-selected to 4 configurations: impingement jet fluidic oscillators (for internal leading edge cooling), reverse film cooling (for pressure surface), sweeping film cooling jets (for suction surface), and trailing edge slot cooling with microchannels. During the 2nd year, the reverse film cooling design was shown to be sub-optimal and work on that topic was halted. The three remaining technologies were integrated into a large scale nozzle guide vane and installed into a low-speed linear cascade facility for further interrogation. Initial results showed the sweeping film cooling jets (on the suction surface) to be the most promising technology compared to a baseline diffusion shaped film hole (777 design). The benefit was particularly evident at high blowing ratios (>1.5) when the 777 coolant film separated from the downstream surface. Benefits were also evident at elevated freestream turbulence levels. The leading edge cooling with unsteady jets was less effective in terms of peak or average cooling – however it was superior to round hole impingement cooling in terms of spatial uniformity. Finally, the trailing edge cooling design with micro-channels was scrapped in favor of a pinned arrangement with centerbody. During the 3rd year, the same three technologies were integrated into a transonic linear cascade for an assessment of compressibility effects. Again, the sweeping film cooling jets proved superior at high blowing ratios while the unsteady leading edge impingement and trailing edge pin-fins with centerbody designs yielded mixed results. Finally, during the 4th and final year, these 3 technologies were integrated into a direct metal laser sintered (DMLS) nozzle guide vane for testing in a high temperature, transonic annular vane cascade. The facility matches the flow temperature, Mach number, and coolant pressure ratios of an actual gas turbine. Before doing this, an additional series of tests were completed to validate a redesigned trailing edge cooling architecture. This final design included a centerbody with triangular pins between the centerbody and the vane external skin. The majority of these triangular pins are fabricated with a 30% gap to the centerbody – reducing their pressure drop considerably while still providing excellent heat transfer augmentation. This additional test campaign required an additional 3-month extension request to complete testing in the high temperature NGV test facility (Turbine Reacting Flow Rig – TuRFR). Testing of the DMLS vane in TuRFR pitted the 3 innovative cooling technologies against more traditional technologies (shaped 777 film hole, round impingement jet, and full pin arrangement in the trailing edge. The sweeping film cooling jets (on the suction surface) showed approximately 15% improvement in overall effectiveness compared to the 777 film hole while the trailing edge showed up to 20% improvement. The leading edge impingement was disappointing with a substantially lower effectiveness than traditional direct impingement. In summary, the study was successful in demonstrating that DMLS-enabled cooling technologies can yield significant gains in cooling performance.

03 NATURAL GAS↗

The influence of random packed column parameters on the liquid holdup and interfacial area

Abstract Carbon dioxide capture via solvent absorption in packed columns has emerged as a potential technology to mitigate coal‐fired power plant CO 2 emissions. Parameters, including packing types, solvent properties, and operating conditions, could potentially affect the packed column CO 2 capture efficiency. To understand the importance of those parameters and help packed column optimization, a design of experiments (DoEs) method was proposed to generate input parameter matrix. Combined with multiphase computational fluid dynamics (CFD), the random packed column parameter influence on the liquid holdup and interfacial area can be efficiently investigated. Surrogate‐based sensitivity analysis shows that the solvent flow rate and contact angle are key factors dictating liquid holdup and interfacial area. On the other hand, solvent viscosity has a marginal impact on the interfacial area. The sensitivity scores were calculated for each input parameter to guide the selection of dimensionless numbers for the liquid holdup and interfacial area correlation development.

42 ENGINEERING↗

Flow dynamics and heat transfer in simplified battery energy storage systems with heated battery modules

Large-scale energy storage systems (ESSs) composed of batteries show promise in addressing current energy challenges, but dissipation of generated heat is important. Here, this paper focuses on buoyant convective flows in simplified ESS battery racks. Natural convection is not generally the primary cooling strategy but can be important in abnormal scenarios where there is module overheat or potentially thermal runaway. We use computational fluid dynamics to investigate the flow dynamics and heat transfer mechanisms in a simplified parameterized rack design. Despite its simplicity, this configuration produces many of the relevant features expected in real ESSs without details of module geometry or hardware, allowing broad conclusions independent of manufacture-specific designs. We start by providing visualizations of the flowfield and measurements of entrainment, heat flux, and pressure. To characterize the dependence on the system parameters, we develop an integral-scale analysis of the average temperature equation to highlight the dominant source terms. We use results from this analysis to derive a steady network model composed of simple algebraic expressions to provide first-order predictions of entrainment through the rack. The network model leads to a linear scaling of the Reynolds number based on convective mass flux with respect to the Grashof number based on the heat source. We deduce empirical relationships that relate the heat exchanged between modules using a surface-averaged Nusselt number as a function of the local Reynolds and Rayleigh numbers. Lastly, we investigate how space between the modules and rack in the spanwise direction creates flow bypass, resulting in different flow pathways.

Battery thermal management↗

Novel method for accurately estimating membrane transport properties and mass transfer coefficients in reverse osmosis

Here, we present a simple and robust method to simultaneously characterize the water and salt permeability (A, B) of reverse osmosis (RO) membranes and mass transfer coefficient (k) in membrane modules. The proposed methodology comprises a set of RO experiments performed at different operating pressures or stages. The measured water and salt fluxes in each stage are simultaneously fitted to the RO transport equations by performing a non-linear regression, using A, B, and k as regression parameters. We first perform a systematic accuracy analysis of the proposed method across the full operational range of RO. The assessment shows that the method accuracy is substantially higher than current methods and increases with number of experimental stages and driving forces. This assessment is used to inform the design of an experimental protocol that minimizes errors in estimated A, B, and k. We then evaluate two commercial RO membranes following the new protocol. For both membranes, A and B parameters decrease by 17% and 15% from the dilute solution to seawater concentrations, whereas the k parameter remains constant. Our study demonstrates that the proposed method, informed by data-driven experimental designs, provides a new approach for accurately characterizing transport phenomenon in membrane processes with feeds of less than 100 g/L total dissolved solids.

36 MATERIALS SCIENCE↗

Statistical description of coalescing magnetic islands via magnetic reconnection

The physical picture of interacting magnetic islands provides a useful paradigm for certain plasma dynamics in a variety of physical environments, such as the solar corona, the heliosheath and the Earth's magnetosphere. In this work, we derive an island kinetic equation to describe the evolution of the island distribution function (in area and in flux of islands) subject to a collisional integral designed to account for the role of magnetic reconnection during island mergers. This equation is used to study the inverse transfer of magnetic energy through the coalescence of magnetic islands in two dimensions. We solve our island kinetic equation numerically for three different types of initial distribution: Dirac delta, Gaussian and power-law distributions. The time evolution of several key quantities is found to agree well with our analytical predictions: magnetic energy decays as $\tilde {t}^{-1}$ , the number of islands decreases as $\tilde {t}^{-1}$ and the averaged area of islands grows as $\tilde {t}$ , where $\tilde {t}$ is the time normalised to the characteristic reconnection time scale of islands. General properties of the distribution function and the magnetic energy spectrum are also studied. Finally, we discuss the underlying connection of our island-merger models to the (self-similar) decay of magnetohydrodynamic turbulence.

Physics↗

Laser wakefield acceleration driven by a discrete flying focus

Laser wakefield acceleration (LWFA) may enable the next generation of TeV-scale lepton colliders. Reaching such energies will likely require multiple LWFA stages to overcome limitations on the energy gain achievable in a single stage. The use of stages, however, introduces challenges such as alignment, adiabatic matching between stages, and a lower average accelerating gradient. Here, we propose a discrete flying focus that can deliver higher energy gain in a single stage, thereby reducing the number of stages required for a target energy. A sequence of laser pulses with staggered focal points and delays drives a plasma wave in which an electron beam experiences a near-constant accelerating gradient over distances beyond those attainable with a conventional pulse. Simulations demonstrate that a discrete flying focus with a total energy of 150 J can transfer 40 GeV per electron to a 50-pC beam in a single 30-cm stage, corresponding to 50 dephasing lengths.

laser wakefield acceleration↗

Recent Progress to Understand and Improve Zeolite Stability in the Aqueous Medium

The work reviewed here attempts to summarize the growing literature on zeolite stability in hot liquid water. This required to first establish the nature, structure and interactions of the active sites in Brønsted and Lewis acidic microporous materials in the presence of liquid water. This understanding was then transferred to zeolite stability and catalyst deactivation. While early results correctly established Si–O–Si hydrolysis as the dominant pathway compared to the Si–O–Al hydrolysis observed in steaming, it also focused extensively on the positive role of framework and extra-framework Al in stabilizing zeolites. However, stability was instead found to more directly correlate with the number of internal structural defects and intraporous water concentration. Stabilization protocols for Brønsted acidic zeolites are described in detail. In the case of Lewis acidic zeolites, their inherent hydrophobic behavior (Si/M >100) makes them more resistant towards water, however, issues such as reversible carbonaceous species formation as well as irreversible metal leaching and fouling remain. Finally, we summarize the most important factors in designing robust and efficient zeolite catalysts made to withstand hot liquid water.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Collaborative Research: Improved Efficiency and Coupling of the Radiation Code in the ACME Earth System Model. Final Report

This final report details all work performed on the project by both project partners. This project provided support to properly couple RTE+RRTMGP, a high-performance broadband radiation code, within DOE’s Energy Exascale Earth System Model (E3SM). RTE+RRTMGP is a successor to the RRTMG radiation code, which has been widely accepted for its speed and accuracy by the global modeling community, and has been in use in the NCAR CESM for many years and was implemented in the initial version of E3SM. However, the computational cost of RRTMG remains high relative to other components in part due to its complexity and to its inefficient use of modern optimization strategies, issues that were rectified by the development of RTE+RRTMGP. Many of the accomplishment in this project necessitated significant collaboration with the E3SM development team. One focus of the project was to enhance the code’s optimization on the limited number of emerging computing systems on which the model is expected be used, including Many Integrated Core (MIC) architectures and Graphics Processing Unit (GPU) hardware. We also developed additional capabilities for RTE+RRTMGP that E3SM scientists identified as important for the planned applications of the model. The result of our project was optimization of a key physical component (radiative transfer calculations) of E3SM, directly supporting E3SM’s overarching global modeling objectives. More broadly, this project provided overall advancements in the use of radiative transfer calculations in atmospheric modeling and simulation, particularly for climate.

54 ENVIRONMENTAL SCIENCES↗

Kinetic Modeling and Experimental Studies of Capacitively Coupled Macro- and Microplasmas at Microwave Frequencies

The effect of driving frequency in the range of 13.56 MHz to 73 MHz on electron energy distribution and electron heating modes in a 50 mTorr capacitively coupled argon plasma discharge is studied using 1D-3V particle-in-cell simulations. Calculated electron energy probability functions exhibit three distinct temperatures for low-, mid-, and high-energy electrons at all the studied driving frequencies. When compared to published experimental data, the calculated probability functions show a reasonable agreement for the energy range resolved in the measurements (about 2 eV to 10 eV). Discrepancies due to limitations in experimental energy resolution outside this range lead to differences between computational and experimental values of the electron number density determined from the distribution functions, and the predicted effective electron temperature is within 25 % of experimental values. The impedance of the discharge is interpreted in terms of a homogeneous equivalent circuit model and the driving frequency dependence of the inferred combined sheath thickness is found to obey a known, theoretically-derived, power law. The average power transferred from the field to the electrons (electron heating) is computed, and a region of negative heating near the sheath edge, particularly at higher driving frequencies, is identified. Analysis of the electron momentum equation shows that electron inertia, which on temporal averaging would be zero in a linear regime, is responsible for negative values of power deposition near the sheath edge at high driving frequencies due to the highly nonlinear behavior of the discharge.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Universal correlation for falling film evaporation on a horizontal plain tube

Falling film evaporators are widely used in many industrial sectors, such as desalination, refrigeration & air-conditioning, and chemical processes. The heat transfer correlations suitable for wider operating conditions and various refrigerants are useful for designing falling film evaporators. Although many researchers developed the correlation for their own experimental data, there is a limited universal correlation for falling film evaporators. In addition, the dry-out effects were not considered in the available universal correlations. Here, therefore, this study proposes a new correlation for falling film evaporation on a single horizontal plain tube, which includes nucleate boiling, film evaporation, and dry-out effects. The proposed correlation covers a wider range of operating conditions (Heat flux is of 2.5–168kWm -2 , and film Reynolds number is up to 3500), various refrigerants (R134a, R245fa, R1234ze(E), R123, R32, R410A, R290, and R600a), and the large number of experimental data (1101 data in total). The proposed correlation is validated against the available standard correlation with regard to mean absolute deviation (MAD) and R 2 values. The MAD of the new correlation is about 10%, respectively, which is the lowest among other correlations. Similarly, the R 2 showed a value of 0.92, which is the highest compared to the existing correlations. A simplified correlation is also proposed.

42 ENGINEERING↗

Coherent high-power RF wakefield generation by electron bunch trains in a metamaterial structure

In this paper, we present an experimental study of coherent high-power wakefield generation in a metamaterial (MTM) structure at 11.7 GHz by 65 MeV electron bunch trains at the Argonne Wakefield Accelerator (AWA), following a previous experiment, the Stage-I experiment, at the AWA. Both the Stage-II experiment, reported in this paper, and the Stage-I experiment were conducted using MTM structures, which are all-metal periodic structures with the period being much smaller than the wavelength. Differences between the two experiments include (1) structure length (Stage-I 8 cm and Stage-II 20 cm); (2) number of bunches used to excite the structure (Stage-I with two bunches, up to 85 nC of total charge; Stage-II with eight bunches, up to 224 nC of total charge); and (3) highest peak power measured (Stage-I 80 MW in a 2 ns pulse and Stage-II 380 MW in a 10 ns pulse). High-power radio frequency pulses were generated by reversed Cherenkov radiation of the electron beam due to the negative group velocity in the MTM structures. Because the radiation is coherent, a train of bunches with a proper spacing can build up to achieve a high peak power. The observed output power levels are very promising for future applications in direct collinear wakefield acceleration or in transfer to a second accelerator for two-beam acceleration.

36 MATERIALS SCIENCE↗