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DOE OSTI2020

Impact of the Cathode Pt Loading on PEMFC Contamination by Several Airborne Contaminants

Proton exchange membrane fuel cells (PEMFCs) with 0.1 and 0.4 mg Pt cm -2 cathode catalyst loadings were separately contaminated with seven organic species: Acetonitrile, acetylene, bromomethane, iso-propanol, methyl methacrylate, naphthalene, and propene. The lower catalyst loading led to larger cell voltage losses at the steady state. Three closely related electrical equivalent circuits were used to fit impedance spectra obtained before, during, and after contamination, which revealed that the cell voltage loss was due to higher kinetic and mass transfer resistances. A significant correlation was not found between the steady-state cell voltage loss and the sum of the kinetic and mass transfer resistance changes. Major increases in research program costs and efforts would be required to find a predictive correlation, which suggests a focus on contamination prevention and recovery measures rather than contamination mechanisms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1987

Solar cycle invariance in solar wind proton temperature relationships

The relationships between solar wind proton temperature and velocity and between temperature and momentum flux density at 1 AU are examined using National Space Science Data Center IMP 8 solar wind data obtained from late 1984 to early 1985. These relationships are compared with similar ones obtained from a variety of solar wind data spanning 14 years, from 1966 to 1980. It is found that these relationships, particularly the one between temperature and velocity, are very stable over the solar cycles from which these data were drawn. This suggests that the basic physical processes which accelerate and heat the solar wind have remained unchanged for the last 20 years.

Lopez, R. E.↗

DOE OSTI2022

The Contribution of Proton-Donor pKa on Reactivity Profiles of [FeFe]-hydrogenases

The [FeFe]-hydrogenases are enzymes that catalyze the reversible activation of H 2 coupled to the reduction–oxidation of electron carriers. Members of the different taxonomic groups of [FeFe]-hydrogenases display a wide range of preference, or bias, for H 2 oxidation or H 2 production reactions, despite sharing a common catalytic cofactor, or H-cluster. Identifying the properties that control reactivity remains an active area of investigation, and models have emerged that include diversity in the catalytic site coordination environments and compositions of electron transfer chains. The kinetics of proton-coupled electron transfer at the H-cluster might be expected to be a point of control of reactivity. To test this hypothesis, systematic changes were made to the conserved cysteine residue that functions in proton exchange with the H-cluster in the three model enzymes: CaI, CpII, and CrHydA1. CaI and CpII both employ electron transfer accessory clusters but differ in bias, whereas CrHydA1 lacks accessory clusters having only the H-cluster. Changing from cysteine to either serine (more basic) or aspartate (more acidic) modifies the sidechain pKa and thus the barrier for the proton exchange step. The reaction rates for H 2 oxidation or H 2 evolution were surveyed and measured for model [FeFe]-hydrogenases, and the results show that the initial proton-transfer step in [FeFe]-hydrogenase is tightly coupled to the control of reactivity; a change from cysteine to more basic serine favored H 2 oxidation in all enzymes, whereas a change to more acidic aspartate caused a shift in preference toward H 2 evolution. Overall, the changes in reactivity profiles were profound, spanning 10 5 in ratio of the H 2 oxidation-to-H 2 evolution rates. The fact that the change in reactivity follows a common trend implies that the effect of changing the proton-transfer residue pKa may also be framed as an effect on the scaling relationship between the H-cluster di(thiolmethyl)amine (DTMA) ligand pKa and E m values of the H-cluster. Experimental observations that support this relationship, and how it relates to catalytic function in [FeFe]-hydrogenases, are discussed.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2024

Tuning Perovskites’ Hydration-Induced Chemical Expansion with Octahedral Tilt Angles

Hydration-induced strains in proton-conducting oxides compromise chemo-mechanical stability when these materials are applied in protonic ceramic electrochemical cells. Here, to develop design principles for zero-strain materials, we systematically studied the hydration coefficients of chemical expansion (CCEs) in perovskite (Sr, Ba)(Ce, Zr, Y)O 3–x solid solutions with in situ dilatometry and thermogravimetric analysis in the range of 430–630 °C. By including and decoupling a wide range of tolerance factors and lattice parameters, we were able to identify a minimum in hydration CCEs (0–0.02) at intermediate tolerance factor values (t ≈ 0.95). Conversely, despite expectations of lower CCEs in larger unit cells, no general trend in CCE versus lattice parameter was found, and opposite trends could be seen for Sr(Ce, Zr, Y)O 3–x versus Ba(Ce, Zr, Y)O 3–x separately. In situ neutron diffraction (ND) enabled atomistic insight. Upon decreasing t, chemical strain anisotropy increased, but this trend did not match the U-shaped dependence of macroscopic CCEs on t. Instead, perovskites with intermediate t, hosting intermediate octahedral tilt angles in the nominally dry state, underwent the largest change in the B–O–B angles during hydration. Accommodating hydration through decreasing B–O–B angles is beneficial because it does not result in large lattice parameter changes. We propose an intermediate tolerance factor as a simple structural descriptor to enable near-zero hydration strains in proton-conducting perovskites.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Analysis of a Prototype Multi-Detector Fast-Neutron Radiography Panel

A multi-detector fast neutron radiography panel was built using the previous work on scalable neutron radiography using the IDEAS ROSSPAD readout module. A new aluminum housing was built to accommodate a large number of detectors tiled together. Additional changes to startup and processing code were made to operate the detector as one cohesive unit. Spatial resolution of the full panel using Cs-137 gammas was reported to be 0.42 line pairs per centimeter at 90% MTF and 2.09 line pairs per centimeter at 10% MTF. Here, three neutron radiographs generated using a Cf-252 fission neutron source were used to determine the spatial resolution of the panel for neutrons. The experiments had 90% MTF values of 0.24, 0.3, and 0.27 line pairs per centimeter and 10% MTF values of 1.30, 1.46, and 1.40 line pairs per centimeter. An example neutron radiograph was also used to prove that the radiography panel can perform true neutron radiography.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2022

Radiographic Imaging and Tomography

Radiographic imaging and tomography (RadIT) come in many flavors such as X-ray imaging and tomography (IT), proton IT, neutron IT, muon IT, neutrino IT, etc. We identify five RadIT themes: Physics, Sources, Detectors, Methods, and Data Science, which are integral parts of image interpretation and three-dimensional (3D) tomographic reconstruction. Traditionally, RadIT have been driven by medicine, non-destructive testing, material sciences, and security applications. The latest thrusts of growth come from automation, machine vision, additive manufacturing and virtual reality (‘metaverse’). The five RadIT themes parallel their counterparts in optical IT. Synergies among different forms of RadIT and with optical IT motivate further advances towards multi-modal IT and quantum IT.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

NASA NTRS1991

The AE-8 trapped electron model environment

The machine sensible version of the AE-8 electron model environment was completed in December 1983. It has been sent to users on the model environment distribution list and is made available to new users by the National Space Science Data Center (NSSDC). AE-8 is the last in a series of terrestrial trapped radiation models that includes eight proton and eight electron versions. With the exception of AE-8, all these models were documented in formal reports as well as being available in a machine sensible form. The purpose of this report is to complete the documentation, finally, for AE-8 so that users can understand its construction and see the comparison of the model with the new data used, as well as with the AE-4 model.

Vette, James I.↗

NASA NTRS2003

Improving the Science Observing Efficiency of the Chandra X-ray Observatory via Chandra Radiation

The Chandra X-ray Observatory (CXO), NASA' latest "Great Observatory", swas launched on July 23, 1999 and reached its final orbit on August 7, 1999. The CXO is in a highly elliptical orbit, approximately 140,000 km x 10,000 km, and has a period of approximately 63.5 hours (approx. 2.65 days). It transits the Earth's Van Allen belts once per orbit during which no science observations can be performed due to the high radiation environment. The Chandra X-ray Observatory Center currently uses the National Space Science Data Center's "near Earth" AP-8/AE-8 radiation belt model to predict the start and end times of passage through the radiation belts. Our earlier analysis demonstrated that our implementation of the AP-8/AE-8 model (a simple dipole model of the Earth's magnetic field) does not always give sufficiently accurate predictions of the start and end times of transit of the Van Allen belts. This led to a change in our operating procedure whereby we "padded" the start and end times of transit by 10 kiloseconds (ks) so that ACIS, the primary science instrument on-board Chandra, would not be exposed to the "fringes" of the Van Allen belts on ingress and egress for any given transit. This additional 20 ks per orbit during which Chandra is unable to perform science observations sums to approximately 3 Ms of "lost" science time per year and therefore reduces the science observing efficiency of the Observatory. To address the need for a higher fidelity radiation model appropriate for the Chandra orbit, the Chandra Radiation Model (CRM) was developed. The CRM is an ion model for the outer magnetosphere and is based on data from the EPIC/ICS instrument on-board the Geotail satellite as well as data from the CEPPAD/IPS instrument on-board the Polar satellite. With the production and implementation of the CRM, we present the results of a study designed to investigate the science observing time that may be recovered by using the CRM as a function of the additional low-energy proton exposure to ACIS.

Virani, Shanil↗

NASA NTRS2003

Improving the Science Observing Efficiency of the Chandra X-Ray Observatory via the Chandra Radiation Model

The Chandra X-ray Observatory (CXO), NASA's latest "Great Observatory", was launched on July 23, 1999 and reached its final orbit on August 7, 1999. The CXO is in a highly elliptical orbit, approximately 140,000 km x 10,000 km, and has a period of approximately 63.5 hours (N 2.65 days). It transits the Earth's Van Allen belts once per orbit during which no science observations can be performed due to the high radiation environment. The Chandra X-ray Observatory Center currently uses the National Space Science Data Center's "near Earth" AP-8/AE-8 radiation belt model to predict the start and end times of passage through the radiation belts. Our earlier analysis demonstrated that our implementation of the AP-8/AE-8 model (a simple dipole model of the Earth's magnetic field) does not always give sufficiently accurate predictions of the start and end times of transit of the Van Allen belts. This led to a change in our operating procedure whereby we "padded" the start and end times of transit by 10 kiloseconds (ks) so that ACIS, the primary science instrument on-board Chandra, would not be exposed to the "fringes" of the Van Allen belts on ingress and egress for any given transit. This additional 20 ks per orbit during which Chandra is unable to perform science observations sums to approximately 3 Ms of "lost" science time per year and therefore reduces the science observing efficiency of the Observatory. To address the need for a higher fidelity radiation model appropriate for the Chandra orbit, the Chandra Radiation Model (CRM) was developed. The CRM is an ion model for the outer magnetosphere and is based on data from the EPIC/ICS instrument on-board the Geotail satellite as well as data from the CEPPAD/IPS instrument on-board the Polar satellite. With the production and Implementation of the CRM, we present the results of a study designed to investigate the science observing time that may be recovered by using the CRM as a function of the additional low-energy proton exposure to ACIS.

Virani, Shanil↗

NASA NTRS2013

Sampling and Analysis of Impact Crater Residues Found on the Wide Field Planetary Camera-2 Radiator

After nearly 16 years in low Earth orbit (LEO), the Wide Field Planetary Camera-2 (WFPC2) was recovered from the Hubble Space Telescope (HST) in May 2009, during the 12 day shuttle mission designated STS-125. The WFPC-2 radiator had been struck by approximately 700 impactors producing crater features 300 microns and larger in size. Following optical inspection in 2009, agreement was reached for joint NASA-ESA study of crater residues, in 2011. Over 480 impact features were extracted at NASA Johnson Space Center's (JSC) Space Exposed Hardware clean-room and curation facility during 2012, and were shared between NASA and ESA. We describe analyses conducted using scanning electron microscopy (SEM) - energy dispersive X-ray spectrometry (EDX): by NASA at JSC's Astromaterials Research and Exploration Science (ARES) Division; and for ESA at the Natural History Museum (NHM), with Ion beam analysis (IBA) using a scanned proton microbeam at the University of Surrey Ion Beam Centre (IBC).

Kearsley, A. T.↗

NASA NTRS1992

A convected kappa distribution model for hot ions in the Jovian magnetodisc

Hot ion angular anisotropies measured by the Low Energy Charged Particle (LECP) instrument during the Voyager 2 encounter with the Jovian dayside outer magnetosphere (60-30 RJ) have been fitted to a 2 species convected kappa distribution function using a nonlinear least squares technique. The resulting parameters are well constrained by the data. The heavy ion species was assumed to be either sulfur or oxygen of unknown charge. The light species was assumed to be protons. The bulk flow speeds deduced from the model were found, contrary to some theories, to increase with increasing radial distance from Jupiter within the radial region addressed, remaining a substantial fraction (0.6) of the rigid corotation speed. Agreement with the averaged Voyager Plasma Science results was obtained near 30 RJ. The core Maxwellian temperature of the heavy ion distribution functions (30-100 keV) increased with increasing radial distance, following the trend anticipated from the corotation pickup of heavy ions. The proton temperature (20 keV) remained nearly constant.

Kane, M.↗

DOE OSTI2024

Proton Quenching in Rare-Earth Inorganic Scintillators: GAGG:Ce and YSO:Ce

Scintillator detectors are an integral component of radiation detection systems for a variety of applications such as medical imaging, accelerator diagnostics, and space science. Typically, a scintillator detector’s response is characterized using gamma sources to understand the detection response to different types of radiation, including charged particle detection. However, there exists a nonlinearity of the amount of light produced from an incident gamma ray of specific energy and the light produced from an incident charged particle of the same energy. This important effect, known as quenching, must be accounted for to interpret energies from charged particles incident on detectors. In this article, we present results of quenching parameterization for two types of cerium-doped inorganic scintillators, Y2SiO5:Ce (YSO:Ce) and Gd3Al2Ga3O12:Ce (GAGG:Ce). We measured the light output from incident proton energies from 1 to 25 MeV using a 3-MV tandem accelerator and two reactions: Au(p,p)Au and 3He(d,p)⁴He. Using gamma-ray sources to calibrate the detectors, we compared the measured electron-equivalent energy versus the incident energy expected. Using an adaptation of the Birks semi-empirical formula, we extracted the Birks parameter (kB) to understand quenching. For one of the GAGG:Ce samples, the kB parameter of 0.0072 [g cm-2 MeV-1] is comparable to a similar study where the value of kB was 0.0065 [g cm-2 MeV-1]. For YSO:Ce, no other kB values were found in the literature. Three different types of GAGG:Ce were used to collect measurements of kB as a function of dopant concentration.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2021

Advanced focusing system for secondary electrons in a bunch shape monitor

Non-destructive measurements of longitudinal beam profile in non-relativistic hadron accelerators are usually performed with Bunch Shape Monitors that utilize secondary electron emission to reproduce the shape of a primary ion beam. The existing devices, however, have poor electron collection efficiency from the wire and are limited to one dimensional measurements of the phase coordinate. Here, we present the development of a bunch shape monitor with improved performance for proton beams to be used in the Spallation Neutron Source accelerator. This improvement was achieved by adding focusing optics between the wire and the entrance slit, which will also allow measurements over a much higher dynamic range. Here we present the design, simulation and experimental test results of the developed new electron beam guidance system for the existing SNS bunch shape monitor that allowed significant improvement in the collection efficiency.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2025

Probing the proton exchange kinetics of BaZr 0.1 Ce 0.7 Y 0.1 Yb 0.1 O 3− δ ceramic electrolyte by operando diffuse reflectance infrared Fourier transform spectroscopy

Proton exchange kinetics plays an important role in governing the performance of intermediate-temperature protonic ceramic electrolysis cells (PCECs) for hydrogen production. Our understanding of the nature of the surface hydration reaction at the single-cell level, however, remains very limited, hampering further efficiency improvements. Here, in this study, we developed a custom operando diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) platform that operates under high temperature and steam conditions with applied bias. Quantitative investigations of surface H 2 O/D 2 O isotope exchange in a BaZr 0.1 Ce 0.7 Y 0.1 Yb 0.1 O 3−δ (BZCYYb1711) protonic electrolyte-based single cell were conducted under different applied voltages using this DRIFTS platform, to gain molecular-level insight into hydration kinetics. The findings show that the application of an external voltage significantly enhances the surface proton exchange rate, decreasing the apparent activation energy from 29.1 kJ mol −1 at open-circuit voltage (OCV) to 6.8 kJ mol −1 at 1.3 V. In addition, distinct voltage-induced spectral shifts in O–D vibrations point to dynamic changes in surface hydration. These findings demonstrate a sensitive spectroscopic platform for probing interfacial proton processes and reveal strong electrochemical control over surface proton kinetics, offering new opportunities for probing electrolyte hydration behavior in PCECs.

36 - MATERIALS SCIENCE↗

DOE OSTI2025

Simulation and measurement of the dynamic strain response in a prototypical spallation target

The Second Target Station (STS) at the Spallation Neutron Source (SNS) will address emerging scientific challenges by providing a source of intense cold neutrons to instruments optimized for this source. The STS target will use rotating tungsten blocks and will receive 1.3 GeV proton beam pulses from the SNS accelerator at a repetition rate of 15 Hz. The facility life is planned for 40 years, and each target assembly life is expected to be approximately 10 years. An accurate strain prediction is then critical for fatigue life assessment of STS target blocks because they will be subject to approximately 10 8 beam pulses per lifetime. As an R&D activity, the Los Alamos Neutron Science Center (LANSCE) Weapons Neutron Research (WNR) Target 2 (Blue Room) facility was used to test the strain response of prototypical target blocks to the thermal shock of a proton pulse. The blue room was well suited for a pulsed proton beam impact test of subscale STS target blocks; the 800 MeV proton energy is approximately 60 % of the 1.3 GeV proton energy expected from the SNS accelerator to the STS. The LANSCE Proton Storage Ring (PSR) and SNS are both short-pulse proton beam sources with nominal pulse widths of 250 ns and 661 ns, respectively, so the energy deposition in the target occurs in <1 μs pulse duration. Strain measurements on the outer surface of three target blocks (bare tungsten, tantalum-clad tungsten, niobium-clad tungsten) were recorded for comparison against neutronics and structural simulations. In conclusion, this experiment and the supporting simulations satisfied the following primary research goals for the STS target.

Dynamic strain response↗

DOE OSTI2023

Recent H - ion source research and development at the Oak Ridge National Laboratory

The U.S. Spallation Neutron Source (SNS) is a state-of-the-art neutron scattering facility delivering the world's most intense pulsed neutron beams to a wide array of instruments which are used to conduct investigations in many fields of science and engineering. Neutrons are produced from spallation of liquid Hg by bombardment of short (~1 μs), intense (~35 A) pulses of protons delivered at 60 Hz by a storage ring which is fed by a high-intensity, ~1 GeV H - LINAC. This facility has operated almost continuously since 2006, with ion source performance increasing over those years, and currently providing 50–60 mA of H - ions with a duty-factor of 6% for maintenance-free runs of several months with near 100% availability. Ion source research and development at ORNL has played a key role in enabling and supporting this success: this report provides an update on some of the ongoing ion source research and development efforts which have been undertaken since the previous Negative Ion Beams and Sources (NIBS) conference in 2020. These include significant improvements to H - beam current by extraction from a larger source outlet aperture and improvements to the electron dumping system which should eliminate the gradual loss of electrode voltage over the course of a run which has occasionally impacted SNS operations. Improvement and simplification of the plasma ignition system for the external antenna ion source, a long-standing problem, was also realized. Lastly, RF coupling efficiency was measured for both the SNS internal and external antenna ion sources.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2023

Fundamental studies of thermal and electrical transport in microporous metal-organic frameworks

In this work, we established porous metal-organic frameworks (MOFs) as designer conductors of electrons and ions relevant to fundamental research and technological applications. MOFs are porous, crystalline materials composed of organic linkers and inorganic nodes. While most MOFs are insulating with respect to ionic and electronic charge carriers, a number of exceptions have been reported in recent years. Electrically conductive MOFs are highly attractive for applications including electrical energy storage, chemiresistive sensing, and optoelectronics because of their high surface areas and tunable chemical properties. Ion-conducting MOFs are desirable for the synthetically tunable size, shape, and polarity of their pore environments, allowing for the tailored development of solid state electrolytes for metal-ion batteries. We developed systematic strategies for the design of MOFs that conduct ions and electrons. For each objective, we leveraged the versatile chemistry of these materials to obtain frameworks with targeted properties towards electronic or ionic charge carriers. We studied the factors that govern electrical transport in MOFs in order to gain fundamental knowledge of this emerging class of materials. We took several approaches to tackle this problem from multiple angles. Namely, we synthesized and characterized new frameworks, investigated post-synthetic modifications to enhance conductivity, and correlated theory and experiment to uncover new mechanistic findings. These results, which put forth new design principles for conductive MOFs, move the field toward one of the DOE Basic Energy Sciences Grand Challenges: to “design and perfect atom- and energy-efficient synthesis of revolutionary new forms of matter with tailored properties.” In addition to investigating the movement of electrons in MOFs, we also studied the movement of other charged species in MOFs, such as protons, lithium, and magnesium. Proton-conducting frameworks could be appealing materials for solid state electrolytes in fuel cells. In addition, they contain crystallographically defined proton-conducting channels, in contrast with state-of-the-art polymer membranes such as Nafion, which are amorphous. Controlling pore size and polarity in MOFs can thus shed light on proton and other ion transport mechanisms, ultimately enabling the design of more advanced electrolyte materials and potentially novel electrical energy storage materials.

36 MATERIALS SCIENCE↗

NASA NTRS2002

A method for calculating proton-nucleus elastic cross-sections

Recently [Nucl. Instr. and Meth. B 145 (1998) 277; Extraction of in-medium nucleon-nucleon amplitude from experiment, NASA-TP, 1998], we developed a method of extracting nucleon-nucleon (N-N) cross-sections in the medium directly from experiment. The in-medium N-N cross-sections form the basic ingredients of several heavy-ion scattering approaches including the coupled-channel approach developed at the NASA Langley Research Center. We investigated [Proton-nucleus total cross-sections in coupled-channel approach, NASA/TP, 2000; Nucl. Instr. and Meth. B 173-174 (2001) 391] the ratio of real to imaginary part of the two body scattering amplitude in the medium. These ratios are used in combination with the in-medium N-N cross-sections to calculate proton-nucleus elastic cross-sections. The agreement is excellent with the available experimental data. These cross-sections are needed for the radiation risk assessment of space missions. c2002 Elsevier Science B.V. All rights reserved.

NASA Center LaRC↗