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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 55 records · Page 3

A Three–Dimensional Nanoscale View of Electrocatalyst Degradation in Hydrogen Fuel Cells

The loss of platinum (Pt) electrochemically active surface area (ECSA) is a critical degradation mode that often becomes a limiting factor for heavy-duty proton exchange membrane fuel cell vehicles. High surface area carbon supports have been shown to improve Pt dispersion and limit detrimental ionomer-electrocatalyst interactions due to their large interior pore volume. Here, in this work, using automated scanning transmission electron tomography, the degradation of nanoparticles located on the interior versus exterior surfaces of the carbon support is compared following a catalyst-specific accelerated stress test (AST) of 90,000 voltage cycles between 0.6 V to 0.95 V. The results reveal a notable increase in median particle size for both interior and exterior Pt catalyst particles, with a slightly higher increase in particle size distribution and loss of specific surface area for the particles located on the exterior carbon surface. The fraction of Pt nanoparticles that reside within the interior of the carbon support also increased following the AST test, accompanied by evidence of an increase in average carbon mesopore size. Here, the results shed light on the degradation mechanisms affecting electrochemical properties and the enhanced particle accessibility at lower relative humidity.

08 HYDROGEN↗

Investigation of the irradiation effects in additively manufactured 316L steel resulting in decreased irradiation assisted stress corrosion cracking susceptibility

While additive manufacturing (AM) is an area of increasing interest to the nuclear industry, there are significant research and development needs prior to successful implementation of additively manufactured components into reactors. AM steel behaves differently than traditional wrought material, as has been observed in numerous mechanical testing studies. The nuclear industry must also understand the material response to irradiation. This work examines the irradiation damage and the irradiation assisted stress corrosion cracking behavior (IASCC) of both proton irradiated AM and wrought 316L steel. For IASCC testing, specimens were strained to 4% plastic strain in a simulated boiling water reactor environment (288°C, 0.2 µS/cm). Transmission and scanning electron microscopy, confocal microscopy, and X-ray computed tomography were used to examine coupons of the material as well as tensile bars used in the IASCC testing. This work found that the wrought 316L was more susceptible to IASCC than the AM steel, however, some IASCC was observed in the AM steel when tested with the tensile axis parallel to the build direction. Electron microscopy has shown significantly fewer radiation induced voids formed in the AM steel. While the pre-existing pore network in the AM steel may act as a sink to point defects, this is not expected to be the major factor in the reduced swelling observed in the AM steel. The lower density of radiation induced voids was expected to contribute to the IASCC resistance by decreasing the localization of deformation in the irradiated specimens, however, severity of localized deformation in AM steel, measured in dislocation channel spacing and height, was similar or more severe to that found in wrought. In conclusion, the presence of severe cracking in the wrought specimens did not allow for a direct comparison of localized deformation severities between the AM and wrought steel.

Additive manufacturing↗

Development of high-performance roll-to-roll-coated gas-diffusion-electrode-based fuel cells

This study focuses on determining fabrication conditions to create high-performance roll-to-roll-coated (R2R-coated) gas-diffusion electrodes (GDEs) for proton-exchange-membrane fuel cells (PEMFCs). Here, we examine how process conditions influence the distribution of ionomer in the electrode, which is shown to be critical for high performance. Using a combination of Kelvin probe, X-ray photoelectron spectroscopy, and nano-scale X-ray computed tomography we show that formation of an ionomer-rich surface is promoted by using a higher drying rate. We show that R2R-coated GDEs have higher surface ionomer concentration than spray-coated GDEs, which enables these R2R-coated GDEs to not need an additional ionomer overlayer, as is typically the case for spray-coated GDEs. This will reduce the number of processing steps and lower material costs in a manufacturing setting. This work shows that with the appropriate selection of materials, ink formulation, and processing conditions, direct-coated GDEs are a viable pathway for fuel cell manufacturing.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

[18F]Tosyl fluoride as a versatile [18F]fluoride source for the preparation of 18F-labeled radiopharmaceuticals

Abstract Positron emission tomography (PET) is an in vivo imaging technology that utilizes positron-emitting radioisotope-labeled compounds as PET radiotracers that are commonly used in clinic and in various research areas, including oncology, cardiology, and neurology. Fluorine-18 is the most widely used PET-radionuclide and commonly produced by proton bombardment of 18 O-enriched water in a cyclotron. The [ 18 F]fluoride thus obtained generally requires processing by azeotropic drying in order to completely remove H 2 O before it can be used for nucleophilic radiofluorination. In general, the drying step is important in facilitating the radiofluorination reactions and the preparation of 18 F-labeled PET radiotracers. In this communication, we have demonstrated the feasibility of using [ 18 F]tosyl fluoride ([ 18 F]TsF) as a versatile [ 18 F]fluoride source for radiofluorination to bypass the azeotropic drying step, and we have developed a continuous flow solid-phase radiosynthesis strategy to generate [ 18 F]TsF in a form that is excellent for radiofluorination. [ 18 F]TsF shows high reactivity in radiofluorination and provides the features suitable for preparing PET radiotracers on a small scale and exploring novel radiolabeling technologies. Thus, using [ 18 F]TsF as a [ 18 F]fluoride source is a promising strategy that facilitates radiofluorination and provides a convenient and efficient solution for the preparation of 18 F-labeled radiopharmaceuticals that is well matched to the emerging trends in PET imaging technologies.

62 RADIOLOGY AND NUCLEAR MEDICINE↗

Characterization of Porous Transport Layers Towards the Development of Efficient Proton Exchange Membrane Water Electrolysis

The current goals for implementing the hydrogen economy have highlighted a need to further optimize water-splitting technologies for clean hydrogen production. Proton exchange membrane water electrolysis (PEMWE) is a leading technology, but further optimizations of anode materials including the porous transport layer (PTL) and the adjacent catalyst layer (CL) are required to increase overall cell performance and reduce cost. This literature review describes advances in PTL development and characterization, highlighting early PTL characterization work and most common methods including capillary flow porometry and mercury intrusion porometry, optical imaging, neutron and x-ray radiography, and x-ray computed tomography. The article also discusses PTL protective coatings and their characterizations, focusing on platinum group metal (PGM)-based coatings, alternative non-PGM-based coatings, post-treated PTLs, and investigations into thin PGM-based coatings. Furthermore, it highlights the integration of the PTL and the adjacent CL along with associated characterization challenges. Lastly, this review discusses future developments in the characterization needed to improve PEMWE's performance and long-term durability are discussed.

08 HYDROGEN↗

Dried Plum Protects From Radiation-Induced Bone Loss by Attenuating Pro-Osteoclastic and Oxidative Stress Responses

Future space explorations beyond the earths magnetosphere will increase human exposure to space radiation and associated risks to skeletal health. We hypothesize that oxidative stress resulting from radiation exposure plays a major role in progressive bone loss and dysfunction in associated tissue. In animal studies, increased free radical formation is associated with pathological changes in bone structure, enhanced bone resorption, reduced bone formation and decreased bone mineral density, which can lead to skeletal fragility. Our long-term goals are to define the mechanisms and risk of bone loss in the spaceflight environment and to facilitate the development of effective countermeasures. We had previously reported that exposure to low or high-LET radiation correlates with an acute increase in the expression of pro-osteoclastic and oxidative stress genes in bone during the early response to radiation followed by pathological changes in skeletal structure. We then conducted systematic screening for potential countermeasures against bone loss where we tested the ability of various antioxidants to mitigate the radiation-induced increase in expression of these markers. For the screen, 16-week old C57Bl6J mice were treated with a dietary antioxidant cocktail, injectable DHLA or a dried plum-enriched diet (DP). Mice were then exposed to 2Gy 137Cs radiation and one day later, marrow cells were collected and the relevant genes analyzed for expression levels. Among the candidate countermeasures tested, DP was most effective in reducing the expression of genes associated with bone loss. Furthermore, analysis of skeletal structure by microcomputed tomography (microCT) revealed that DP also prevents the radiation-induced deterioration in skeletal microarchitecture as indicated by parameters such as percent bone volume (BVTV), trabecular spacing and trabecular number. We also found that DP has similar protective effects on skeletal structure in a follow-up study using 1 Gy of sequential proton and iron, radiation species relevant to spaceflight. When cultured ex vivo under osteogenic conditions, bone marrow-derived cells from DP-fed animals exhibited increased colony numbers compared to control diet-fed animals. These findings suggest that DP exerts pro-osteogenic effects apart from its previously demonstrated anti-resorptive action, which may be one of the mechanisms underlying its radioprotective effect on bone. In conclusion, a diet enriched in certain types of antioxidants may be useful as an intervention for radiation-induced bone loss.

Bone-loss↗

Revealing the Nanostructure of Mesoporous Fuel Cell Catalyst Supports for Durable, High-Power Performance

Achieving high power performance and durability with low Pt loadings are critical challenges for proton exchange membrane fuel cells. PtCo catalysts developed on new carbon black supports show promise by simultaneously providing good oxygen reduction kinetics and local oxygen transport. We investigate the role of nanoscale morphology in the performance of these catalysts supported on accessible (HSC-e and HSC-f) and conventional (Ketjen Black) porous carbons using 3D electron tomography, nitrogen sorption, and electrochemical performance measurements. We find that the accessible porous carbons have hollow interiors with mesopores that are larger and more numerous than conventional porous carbons. However, mesopore-sized openings (>2 nm width) are too rare to account for significant oxygen transport. Instead we propose the primary oxygen transport pathway into the interior is through 1–2 nm microporous channels permeating the carbon. The increased mesoporosity in the accessible porous carbons results in a shorter diffusion pathlength through constrictive, tortuous micropores in the support shell leading to lower local oxygen transport resistance. In durability testing, the accessible porous carbons show faster rates of electrochemical surface area loss, likely from fewer constrictive pores that would mitigate coarsening, but maintain superior high current density performance at end of test from the improved local oxygen transport.

Electrochemistry↗

Production of Radioisotopes of Scandium for Imaging and Therapy (Final Report)

The theranostic approach is a powerful technique that enables scientists and physicians to diagnose and treat diseases using the same targeting moiety labeled with radionuclides for imaging and therapy. A challenge behind synthesizing and evaluating these theranostic radiopharmaceuticals lies in the production of suitable radionuclides. This study aimed to investigate the production of high radionuclidic purity 43 Sc from enriched [ 46 Ti]TiO 2 for Positron Emission Tomography (PET) and 47 Sc from enriched [ 50 Ti]TiO 2 for targeted radiotherapy, as well as establish a target recycling technique for continued production of these radionuclides. Methods: Targets were prepared with 100 mg of either enriched [ 46 Ti]TiO 2 or [ 50 Ti]TiO 2 , pressed into pellets, and placed into Ta target holders with a 0.127 mm natTi cover foil. The 46 Ti targets were bombarded with 18 MeV protons at 20 µA for 1.5 h, while 50Ti targets were bombarded with 24 MeV protons at 20 µA for 4 or 8 h. The radioscandium nuclides were purified using branched N, N, N’, N’ -tetra-2-ethylhexyldiglycolamide (DGA) resin. The titanium targets were recycled by precipitating the dissolved Ti collected from the column effluent and wash streams, pH adjustment, vacuum filtration, and then drying the solid at 250 °C prior to reforming the target for the subsequent bombardment. The apparent molar activity of the isolated radioscandiums was analyzed by titration with 1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetic acid (DOTA). The relative imaging performance of 18 F, 43 Sc, and 68 Ga were analyzed with PET images acquired with 30-min static scans. Results: The average radioscandium recovery for 43Sc was 91.7 ± 7.4 %, with a radionuclidic purity of 98.8 %. The average recovery of 47Sc was 89.9 ± 3.9 %, with a radionuclidic purity of 90.8%. The average recovery of enriched TiO2 was 96 ± 4.0 %. The highest apparent molar activity for [43Sc]Sc-DOTA was 23.2 GBq/µmol and 3.39 GBq/µmol for [ 47 Sc]Sc-DOTA. The order of PET resolution from highest to lowest was 18 F > 43 Sc > 68 Ga. Conclusions: This work demonstrates the feasibility of using enriched recycled [ 46 Ti]TiO 2 and [ 50 Ti]TiO 2 targets for the production of the 43 Sc and 47 Sc theranostic isotope pair in high purity.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Detectors and diagnostics for multiprobe radiography using high-energy short-pulse lasers

Multiprobe radiography requires the following diagnostic capabilities at minimum: radiographic source diagnostics, spectroscopy, imaging, and tomography diagnostics. Depending on the repetition rate of the radiation sources, the diagnostics may be a single-shot diagnostic, such as photographic (radiochromic and X-ray films for high energy photons) films, or a multiple-shot diagnostic for repetitive source operations, such as a high-speed framing camera. Due to the drastically different detector physics of electrons, photons at different energies (keV to 10s of MeV in the radiography context), heavy ions such as protons, alphas, and neutrons, see, for example, Ref. [1, 2] for an overview, different types or configurations of detectors and constructions may be required for multiprobe radiography applications. Some of the common detector metricsinclude, independent of the particle/photon species, sensitivities or efficiency, energy resolution, spatial or temporal resolutions and others. Some unique detection scenarios arise in a multiprobe radiography setting, for example, crosstalk mitigation and particle identification (ID) when X-ray and higher energy photons, relativistic electrons, neutrons, other hadrons, and heavy particles coexist at the detector location.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Comparative Validation of Realtime Solar Wind Forecasting Using the UCSD Heliospheric Tomography Model

The University of California, San Diego 3D Heliospheric Tomography Model reconstructs the evolution of heliospheric structures, and can make forecasts of solar wind density and velocity up to 72 hours in the future. The latest model version, installed and running in realtime at the Community Coordinated Modeling Center(CCMC), analyzes scintillations of meter wavelength radio point sources recorded by the Solar-Terrestrial Environment Laboratory(STELab) together with realtime measurements of solar wind speed and density recorded by the Advanced Composition Explorer(ACE) Solar Wind Electron Proton Alpha Monitor(SWEPAM).The solution is reconstructed using tomographic techniques and a simple kinematic wind model. Since installation, the CCMC has been recording the model forecasts and comparing them with ACE measurements, and with forecasts made using other heliospheric models hosted by the CCMC. We report the preliminary results of this validation work and comparison with alternative models.

MacNeice, Peter↗

Overview of SoLID

SoLID spectrometer was proposed to fully exploit the potential of JLab 12 GeV energy upgrade. It is a large acceptance detector which can handle very high luminosity. An overview of the rich physics program will be given, which includes number of planned measurements: a multi-dimensional mapping of semi-inclusive DIS asymmetries for tomography of the nucleon in momentum space in the high-x region and precision determination of the tensor charge; a measurement of parity-violating DIS to provide a precision test of the Standard Model, reaching a sensitivity to new physics at 10-20 TeV level; a precision measurement of J/psi photo- and electro-production cross sections in the threshold region to probe the strong color fields in the nucleon and to study the origin of the proton mass. The current status and the plan of the project will be discussed.

Chen, Jian-Ping↗

Stochastic generation of electrolyzer anode catalyst layers

Here, we introduce a stochastic methodology to reproduce the complex pore structure observed in commercial iridium catalyst layers. This method preserves the α pore (pores smaller than 250 nm) and β pore (pores greater than or equal to 250 nm) regions of the catalyst layer. The morphology of the generated materials was validated by comparing the pore size distributions of generated materials against those obtained from commercial materials imaged using x-ray nano computed tomography. We further demonstrate that the pore size distributions of the generated materials are statistically indistinguishable from the imaged catalyst layers, indicating that the stochastic methodology is capable of accurately reproducing catalyst layer morphology. Pore network modelling was conducted on the generated catalyst materials to simulate single-phase permeability, electrical conductivity, and ionic conductivity, and these properties were found to be within experimentally measured ranges for electrolyzer catalyst layers. Additionally, simulations were performed on the generated materials with varying ionomer and iridium catalyst loadings. As the ionomer loading is added, proton conductivity increases exponentially, which demonstrates the importance of optimizing ionomer loading, considering that these effects will be exacerbated in the hydration and temperature conditions of operating electrolyzers. The stochastic material generation method presented in this work is a powerful tool for the development of novel low loading catalyst layers, where the effect of various structural parameters on electrolyzer performance characteristics can be explored.

36 MATERIALS SCIENCE↗

Measurement of the Deeply Virtual Compton Scattering Cross Section from the Proton at 10.6 GeV using the CLAS12 Detector

Deeply Virtual Compton Scattering (DVCS) is an exclusive process that produces a real photon when a lepton scatters from a quark inside a nucleon or a nucleus. Measurement of the DVCS cross section enables the study of the Generalized Parton Distributions (GPD), which plays a central role in understanding the QCD dynamics inside a hadron. Thus, the quark and gluon origin of the nucleon spin and mass can be probed and three-dimensional images of the target nucleon or nucleus can be realized. This thesis presents a cross section analysis of DVCS from the proton in the presence of its background, Bethe-Heitler (BH) process. The CEBAF Large Acceptance Spectrometer for operation at 12 GeV beam energy (CLAS12) collaboration has taken electron-proton scattering data in fall 2018 using a liquid hydrogen target and the 10.6 GeV polarized electron beam from the Continuous Electron Beam Accelerator Facility (CEBAF). The CLAS12 detector is a nearly hermetic fixed-target detector, located in Hall B, Jefferson Lab at Newport News, Virginia. The experimentally determined BH-DVCS cross section is in good agreement with a phenomenological-model based theoretical prediction. The kinematic dependence of the cross section is reported over a wide range. The short-term plan to utilize the results presented here for a thorough tomography study and the long-term plan for GPD studies at future facilities such as the Electron-Ion Collider (EIC) are discussed.

Lee, Sangbaek↗

Physical model and experimental validation of a high temperature proton exchange membrane electrochemical hydrogen pump cell for efficient single-stage extraction of low concentration hydrogen gas

There is interest in valorization of existing natural gas infrastructure to facilitate the co-transportation of hydrogen via blending of hydrogen gas initially at limited concentrations of 1–20 vol% H2 and to subsequently extract hydrogen at fuel cell quality standards (SAE J2719/ISO14687-2). High temperature proton exchange membrane electrochemical hydrogen pump (HT-PEM EHP) based on phosphoric acid doped polybenzimidazole (PA-PBI) exhibits good performance at elevated temperatures (>120 °C), which provides desirable tolerance to non-methane natural gas constituents that are problematic for lower temperature based EHP. To better understand the suitability of the HT-PEM EHP for such gas separation processes, a two-dimensional model of EHP based on PA-PBI was developed. The model is validated for several relevant operating conditions and across cells with differing amounts of phosphoric acid content in the electrodes. Operando micro x-ray computed tomography (CT) imaging of an HT-PEM EHP was used to further validate physical parameters and assumptions of the model. The impacts of pressure, relative humidity of the anode feed, and concentration of feed gases on separation performance are investigated. This study shows that a specific energy of separation of 5.1 kWh/kg H2 at a hydrogen recovery factor (HRF) of 50 vol% can be achieved in a single stage with the EHP, producing fuel cell quality hydrogen purity of 99.99 vol% H2 from a 2 vol% H2/CH4 feed blend, while pressurizing the product H2 at a pressure ratio of 1.3 relative to feed pressure.

Stansberry, John M↗

Single Cobalt Sites Dispersed in Hierarchically Porous Nanofiber Networks for Durable and High-Power PGM-Free Cathodes in Fuel Cells

Increasing catalytic activity and durability of atomically dispersed metal–nitrogen–carbon (M–N–C) catalysts for the oxygen reduction reaction (ORR) cathode in proton-exchange-membrane fuel cells remains a grand challenge. In this study, a high-power and durable Co–N–C nanofiber catalyst synthesized through electrospinning cobalt-doped zeolitic imidazolate frameworks into selected polyacrylonitrile and poly(vinylpyrrolidone) polymers is reported. The distinct porous fibrous morphology and hierarchical structures play a vital role in boosting electrode performance by exposing more accessible active sites, providing facile electron conductivity, and facilitating the mass transport of reactant. The enhanced intrinsic activity is attributed to the extra graphitic N dopants surrounding the CoN 4 moieties. The highly graphitized carbon matrix in the catalyst is beneficial for enhancing the carbon corrosion resistance, thereby promoting catalyst stability. The unique nanoscale X-ray computed tomography verifies the well-distributed ionomer coverage throughout the fibrous carbon network in the catalyst. The membrane electrode assembly achieves a power density of 0.40 W cm –2 in a practical H 2 /air cell (1.0 bar) and demonstrates significantly enhanced durability under accelerated stability tests. The combination of the intrinsic activity and stability of single Co sites, along with unique catalyst architecture, provide new insight into designing efficient PGM-free electrodes with improved performance and durability.

25 ENERGY STORAGE↗

Effect of Engineered Cracks in Catalyst Layers on PEMFC Catalyst Layer Durability

Proton exchange membrane fuel cells (PEMFCs) are expected to play a pivotal role in decarbonizing the transportation sector, and particularly heavy-duty vehicles (HDVs). However, improvements in durability are needed for PEMFCs to compete with state-of-the-art power sources for HDVs. Here, we examine how catalyst layer (CL) cracks that are engineered affect the CL durability by using patterned silicon templates to control the CL crack density at the micrometer scale. Electrochemical analyses show that the initial PEMFC performance is relatively unaffected by crack density, but the performance after durability testing was strongly affected. Specifically, CLs with high crack density showed higher performance relative to CLs without cracks after application of a carbon corrosion accelerated stress test. Electrochemical analyses coupled with X-ray computed tomography and scanning transmission electron microscopy with energy dispersive X-ray spectroscopy showed that the cracks provide shorter oxygen diffusion pathways to reaction sites, leading to decreased oxygen transport resistance. Additionally, we observed that the catalyst durability is unaffected by cracks. Our results provide a mechanistic explanation of the role of cracks in CL durability.

30 DIRECT ENERGY CONVERSION↗

Linking structure to performance: Characterization of porous transport layers for high-pressure water electrolysis

Proton exchange membrane (PEM) water electrolysis is a promising technology to produce cost-efficient hydrogen. PEM electrolyzers offer a large current density range and the ability to operate at differential pressure which can be used to minimize both capital and operational expenditures. However, directly producing pressurized hydrogen at the cathode results in pushing the membrane against the anode porous transport layer (PTL). This can lead to detrimental effects, such as membrane deformation or ruptures, which depend on membrane properties as well as PTL material properties such as pore size, structure, and morphology. In this work, a range of sinter and felt-based commercial PTLs are evaluated for their contributions to the cell's electrochemical and H 2 crossover performance at cathode pressures up to 30 bar. X-ray tomography and post-operando optical microscopy are used to assess the morphology of the PTLs, and the PTL induced deformation experienced by the catalyst coated membrane (CCM), respectively. PTL samples with lower porosity were found to reduce both the cell voltage and the amount of H 2 permeating from the cathode to the anode exhaust, which was ascribed to improved catalyst layer contact and reduced membrane deformation, respectively. The best performing PTLs improved electrolyzer efficiency by ~1.5 kWh/kg H2 . Specifically, 1 kWh/kg H2 was gained due to reducing membrane deformation and decreasing H 2 crossover. The remainder 0.5 kWh/kg H2 were achieved by improving the electrical contact at the electrode/PTL interface which decreased cell voltage.

08 HYDROGEN↗