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DOE OSTI2016

Radioactive Material Inventory Optimization Using the Plutonium-239 Equivalent Curie Methodology

ABSTRACT The purpose of this paper is to provide the technical basis for application of the Plutonium 239 equivalent curies (PEC) concept used to optimize and limit the material-at-risk (MAR) in the Irradiated Materials Characterization Laboratory (IMCL) located at the Materials and Fuels Complex (MFC). The PEC concept offers a method to normalize all radionuclides to a common radiotoxic hazard index that can be summed to a single value. This paper describes the technical approach to applying the PEC concept, documents the weighting factors and specific activities to be utilized in the calculation, and provides an example of the application of the concept to a radionuclide distribution that is representative of materials encountered in the IMCL. The IMCL is operated to provide a dynamic, re-configurable capability to analyze and characterize irradiated or non-irradiated radioactive material samples. The operations unique to the IMCL include sample storage, preparation, and analysis using experiment-specific instrumentation such as, Electron probe micro-analyzer (EPMA), Focused ion beam (FIB), Transmission electron microscope (TEM), and Scanning electron microscope (SEM). The methodology used to characterize the radioactive material inventory enables the IMCL to operate in such a way that complements their capability and program goals without compromising the safety of the worker, co-located worker, or the general public. The PEC concept offers a method in which all radionuclide inventory is normalized to a common radiotoxic hazard index that can be summed to a single value. The PEC concept is useful in the comparison of various material types for hazard categorization and for identifying worst-case and bounding inventory.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2015

Cr(VI) Occurrence and Geochemistry in Water From Public-Supply Wells in California

Hexavalent chromium, Cr(VI), in 918 wells sampled throughout California between 2004 and 2012 by the Groundwater Ambient Monitoring and Assessment Program—Priority Basin Project (GAMA—PBP) ranged from less than the study reporting limit (SRL) of 1 microgram per liter (μg/L) to 32 μg/L. Statewide, Cr(VI) was reported in 31 percent of sampled wells and equaled or exceeded the recently established (2014) California Maximum Contaminant Level (MCL) for Cr(VI) of 10 μg/L in 4 percent of sampled wells. Cr(VI) data collected for regulatory purposes overestimate Cr(VI) occurrence. Ninety percent of chromium was present as Cr(VI), which was detected more frequently and at higher concentrations in alkaline (pH > 8), oxic water, and more frequently in agricultural and urban land uses compared to native land uses. Chemical, isotopic (tritium and carbon-14), and noble-gas data show high Cr(VI) in water from wells in alluvial aquifers in the southern California deserts result from long groundwater-residence times and geochemical reactions such as silicate weathering that increase pH, while oxic conditions persist. High Cr(VI) in water from wells in alluvial aquifers along the west-side of the Central Valley results from high-chromium abundance in source rock eroded to form those aquifers, and areal recharge processes (including irrigation return) that mobilize chromium from the unsaturated zone. Cr(VI) co-occurred with oxyanions having similar chemistry, including vanadium, selenium, and uranium. Cr(VI) was positively correlated with nitrate, consistent with increased concentrations in areas of agricultural land use and mobilization of chromium from the unsaturated zone by irrigation return.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2017

Two-Dimensional Neutronic and Fuel Cycle Analysis of the Transatomic Power Molten Salt Reactor

This status report presents the results from the first phase of the collaboration between Transatomic Power Corporation (TAP) and Oak Ridge National Laboratory (ORNL) to provide neutronic and fuel cycle analysis of the TAP core design through the Department of Energy Gateway for Accelerated Innovation in Nuclear, Nuclear Energy Voucher program. The TAP design is a molten salt reactor using movable moderator rods to shift the neutron spectrum in the core from mostly epithermal at beginning of life to thermal at end of life. Additional developments in the ChemTriton modeling and simulation tool provide the critical moderator-to-fuel ratio searches and time-dependent parameters necessary to simulate the continuously changing physics in this complex system. Results from simulations with these tools show agreement with TAP-calculated performance metrics for core lifetime, discharge burnup, and salt volume fraction, verifying the viability of reducing actinide waste production with this design. Additional analyses of time step sizes, mass feed rates and enrichments, and isotopic removals provide additional information to make informed design decisions. This work further demonstrates capabilities of ORNL modeling and simulation tools for analysis of molten salt reactor designs and strongly positions this effort for the upcoming three-dimensional core analysis.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE OSTI2022

Candidacy Renewal Report for ICERR Designation

The International Atomic Energy Agency (IAEA) has established a designation for an International Centre based on Research Reactors (ICERR). The intention of this designation is to provide a vehicle for IAEA member states to access international research-reactor and ancillary nuclear research and development infrastructure. The U.S. Department of Energy (DOE) has made a commitment to world leadership in the development of advanced nuclear energy, science, and technology. To this end, DOE has established programs and initiatives to enhance this leadership role. ICERR designation constitutes an important step in achieving the DOE vision. DOE, represented by Idaho National Laboratory (INL) and Oak Ridge National Laboratory (ORNL), is submitting this application for re-designation as an IAEA ICERR. Both INL and ORNL have a decades-long and storied history that supports nuclear research, development, and deployment both nationally and internationally. Both have a history of safe and efficient nuclear operations and have demonstrated a track record of international collaboration and cooperation. INL and ORNL are home to two primary and two secondary research reactors. The primary reactors are Advanced Test Reactor at INL, and High-Flux Isotope Reactor at ORNL. Secondary reactors include: Neutron Radiography Reactor at INL, Transient Reactor Test (TREAT) Facility at INL, and INL Advanced Test Reactor: Critical Facility (ATRC). ICERR designation will also include numerous ancillary facilities at both laboratories, including the following: Multiple post-irradiation examination facilities at both INL and ORNL, Radiochemistry hot-cell facilities at ORNL, INL nuclear-fuel-fabrication and materials-science facilities, and INL and ORNL radiological and nuclear analytical capabilities.

99 GENERAL AND MISCELLANEOUS↗

DOE OSTI2022

Improved $^{95}\mathrm{Mo}$ neutron resonance parameters and astrophysical reaction rates

We report improved 95 Mo neutron resonance parameters and reaction rates are important for nuclear astrophysics, testing nuclear models, and nuclear criticality safety. However, despite many previous neutron-capture and total cross-section measurements on this nuclide, there still is much room for improvement as well as several discrepancies. For example, there are very few firm resonance spin and parity assignments; average resonance parameters are available only for each parity, the currently recommended astrophysical reaction rate results in disagreements between stellar models and meteoric isotopic anomalies, and there are substantial disagreements in the neutron-capture cross section at low energies important for nuclear criticality safety. To obtain an improved set of neutron resonance parameters and astrophysical reaction rates for 95 Mo. High-resolution neutron-capture and transmission data were measured at the Oak Ridge Electron Linear Accelerator (ORELA) using highly isotopically enriched 95 Mo samples. The neutron-capture apparatus, data reduction, and analysis were improved so that information contained in the γ-ray cascade following neutron capture were used to assign resonance J π values. Following this, simultaneous analysis of the new neutron-capture and transmission data was used to obtain resonance energies, gamma widths, and neutron widths and their uncertainties to a maximum energy of 10 keV. Accurate neutron-capture cross sections also were obtained for the unresolved resonance region to a maximum energy of 500 keV and, together with the new resonance parameters, used to calculate the astrophysical reaction rates in the temperature range from 5 to 30 keV. A vastly improved set of 95Mo neutron resonance parameters and an astrophysical reaction rate accurate to about 3% were obtained. Firm J π assignments were determined for 261 of the 314 observed resonances. This is a very large improvement over the previously published 32 firm J π assignments for 108 resonances. Also, the number of resonances having both firm J π assignments and Γ γ values was increased by almost a factor of 24—from 11 to 261. Neutron- and total-radiation-width distributions and average resonance spacings, average total radiation widths, and neutron strength functions were obtained for the six different s- and p-wave possibilities. Parameters for the lowest s-wave resonance, which is most important for criticality benchmarks, were obtained with high accuracy. Simple modification of the neutron-capture apparatus and expansion and improvement of data analysis techniques led to a large increase in firm J π assignments for 95 Mo neutron resonances. The resulting astrophysical reaction rate is 20%–30% larger than the currently recommended rate at s-process temperatures, which should lead to better agreement between stellar models and meteoric isotopic anomalies. The neutron-capture cross section at low energies is substantially larger than recommended in the latest evaluation, which is problematical for criticality benchmarks. The average resonance spacing as a function of spin and parity is significantly different from current models. The total-radiation-width distributions are significantly broader than predicted by theory and show significant departures from the expected Gaussian shapes.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2017

Wallula Basalt Pilot Demonstration Project: Post-injection Results and Conclusions

Deep underground geologic formations are emerging as a reasonable option for long-term storage of CO 2 , including large continental flood basalt formations. At the GHGT-11 and GHGT-12 conferences, progress was reported on the initial phases for Wallula Basalt Pilot demonstration test (located in Eastern Washington state), where nearly 1,000 metric tons of CO 2 were injected over a 3-week period during July/August 2013. The target CO 2 injection intervals were two permeable basalt interflow reservoir zones with a combined thickness of ~20 m that occur within a layered basalt sequence between a depth of 830-890 m below ground surface. During the two-year post-injection period, downhole fluid samples were periodically collected during this post-injection monitoring phase, coupled with limited wireline borehole logging surveys that provided indirect evidence of on-going chemical geochemical reactions/alterations and CO 2 disposition. A final detailed post-closure field characterization program that included downhole fluid sampling, and performance of hydrologic tests and wireline geophysical surveys. Included as part of the final wireline characterization activities was the retrieval of side-wall cores from within the targeted injection zones. These cores were examined for evidence of in-situ mineral carbonization. Visual observations of the core material identified small globular nodules, translucent to yellow in color, residing within vugs and small cavities of the recovered basalt side-wall cores, which were not evident in pre-injection side-wall cores obtained from the native basalt formation. Characterization by x-ray diffraction identified these nodular precipitates as ankerite, a commonly occurring iron and calcium rich carbonate. Isotopic characterization (δ 13 C, δ 18 O) conducted on the ankerite nodules indicate a distinct isotopic signature that is closely aligned with that of the injected CO 2 . Both the secondary mineral nodules and injected CO 2 are measurably different from the isotopic content of basalt, injection zone groundwater and for naturally occurring calcite. Final post-injection wireline geophysical logging results also indicate the presence of free-phase CO 2 at the top of the two injection interflow zones, with no vertical migration of CO 2 above the injection horizons. Furthermore, these findings are significant and demonstrate the feasibility of sequestering CO 2 in a basalt formation.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2015

Current status of tritium calorimetry at TLK

Inside a tritium facility, calorimetry is an important analytical method as it is the only reference method for accountancy (it is based on the measurement of the heat generated by the radioactive decay). Presently, at Tritium Laboratory Karlsruhe (TLK), 4 calorimeters are in operation, one of isothermal type and three of inertial guidance control type (IGC). The volume of the calorimeters varies between 0.5 and 20.6 liters. About two years ago we started an extensive work to improve our calorimeters with regard to reliability and precision. We were forced to upgrade 3 of our 4 calorimeters due to the outdated interfaces and software. This work involved creating new LabView programs driving the devices, re-tuning control loops and replacing obsolete hardware components. In this paper we give a review on the current performance of our calorimeters, comparing it to recently available devices from the market and in the literature. We also show some ideas for a next generation calorimeter based on experiences with our IGC calorimeters and other devices reported in the literature. (authors)

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2015

Post-Irradiation Examination of 237Np Targets for 238Pu Production

Oak Ridge National Laboratory is recovering the US 238 Pu production capability and the first step in the process has been to evaluate the performance of a 237 Np target cermet pellet encased in an aluminum clad. The process proceeded in 3 steps; the first step was to irradiate capsules of single pellets composed of NpO 2 and aluminum power to examine their shrinkage and gas release. These pellets were formed by compressing sintered NpO 2 and aluminum powder in a die at high pressure followed by sintering in a vacuum furnace. Three temperatures were chosen for sintering the solution precipitated NpO 2 power used for pellet fabrication. The second step was to irradiate partial targets composed of 8 pellets in a semi-prototypical arrangement at the two best performing sintering temperatures to determine which temperature gave a pellet that performed the best under the actual planned irradiation conditions. The third step was to irradiate ~50 pellets in an actual target configuration at design irradiation conditions to assess pellet shrinkage and gas release, target heat transfer, and dimensional stability. The higher sintering temperature appeared to offer the best performance after one cycle of irradiation by having the least shrinkage, thus keeping the heat transfer gap between the pellets and clad small minimizing the pellet operating temperature. The final result of the testing was a target that can meet the initial production goals, satisfy the reactor safety requirements, and can be fabricated in production quantities. The current focus of the program is to verify that the target can be remotely dissembled, the pellets dissolved, and the 238 Pu recovered. Tests are being conducted to examine these concerns and to compare results to code predictions. Once the performance of the full length targets has been quantified, the pellet 237 Np loading will be revisited to determine if it can be increased to increase 238 Pu production.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2016

An investigation of MCNP6.1 beryllium oxide S(α, β) cross sections

Here, in MCNP6.1, materials are constructed by identifying the constituent isotopes (or elements in a few cases) individually. This list selects the corresponding microscopic cross sections calculated from the free-gas model to create the material macroscopic cross sections. Furthermore, the free-gas model and the corresponding material macroscopic cross sections assume that the interactions of atoms do not affect the nuclear cross sections.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2015

Final Report for EPSCoR Implementation Award DE-FG02-08ER46528 to University of Tennessee

With the completion of the Spallation Neutron Source (SNS) and upgrading of the High-Flux Isotope Reactor (HFIR) at the Oak Ridge National Laboratory (ORNL) the state of Tennessee now leads the world in the capability of neutron scattering research. This project aimed at directing the great impact of these facilities to researchers in the EPSCoR states, Tennessee in particular, by creating a research collaboration network around these facilities. The plan consisted of two parts: (1) Direct effort to increase the user base through the travel fellowship for graduate students and faculty from the EPSCoR states to use the neutron facilities at the ORNL, and through workshops and schools on the application of neutron scattering, and (2) Research collaboration among the core participants from UTK, ORNL and other states. The EPSCoR Travel Fellowship Program has supported over 300 distinct and 600 cumulative neutron facility users and over 250 workshop participants, with the total of nearly 600 distinct recipients. This program has been highly popular particularly among young faculty members who often have difficulty in raising travel funds, and enabled participation of young graduate students to neutron research. This program has been the foundation of this project. We supported several educational workshops, organized one (“neutrons for novice”) by ourselves each year, targeting non-users of neutron scattering. These efforts significantly contributed to expand the neutron user base among the EPSCoR states. The core research targeted condensed matter physics and soft matter sciences. The core research groups participating in this project include not only researchers from Tennessee but those from Kansas, South Carolina, Puerto Rico and Louisiana, making this project a national, rather than regional, enterprise. Collaborations that were seeded by this project have grown into two major projects, one in materials science (irradiation effects on high-entropy alloys) and the other in soft matter sciences (bio-membranes). Through this project we promoted the use of neutron scattering, particularly in biological and life sciences and in energy sciences, and facilitated the DOE investment in this field to impact wide fields of science and engineering. This project was administered through the Joint Institute for Neutron Sciences (JINS) of the University of Tennessee (UT) and ORNL. JINS is jointly supported by both UT and ORNL, and participate in organizing workshops and schools to promote the use of neutron scattering.

36 MATERIALS SCIENCE↗

DOE OSTI2015

SU-E-P-05: Electronic Brachytherapy: A Physics Perspective On Field Implementation

Purpose: We want to summarize our experience implementing a successful program of electronic brachytherapy at several dermatology clinics with the help of a cloud based software to help us define the key program parameters and capture physics QA aspects. Optimally developed software helps the physicist in peer review and qualify the physical parameters. Methods: Using the XOFT™ Axxent™ electronic brachytherapy system in conjunction with a cloud-based software, a process was setup to capture and record treatments. It was implemented initially at about 10 sites in California. For dosimetric purposes, the software facilitated storage of the physics parameters of surface applicators used in treatment and other source calibration parameters. In addition, the patient prescription, pathology and other setup considerations were input by radiation oncologist and the therapist. This facilitated physics planning of the treatment parameters and also independent check of the dwell time. From 2013–2014, nearly1500 such calculation were completed by a group of physicists. A total of 800 patients with multiple lesions have been treated successfully during this period. The treatment log files have been uploaded and documented in the software which facilitated physics peer review of treatments per the standards in place by AAPM and ACR. Results: The program model was implemented successfully at multiple sites. The cloud based software allowed for proper peer review and compliance of the program at 10 clinical sites. Dosimtery was done on 800 patients and executed in a timely fashion to suit the clinical needs. Accumulated physics data in the software from the clinics allows for robust analysis and future development. Conclusion: Electronic brachytherapy implementation experience from a quality assurance perspective was greatly enhanced by using a cloud based software. The comprehensive database will pave the way for future developments to yield superior physics outcomes.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2020

Radiological Monitoring Plan for the Oak Ridge Y-12 National Security Complex: Surface Water

DOE Order 458.1 requires that dose estimates consider contributions from all facilities. In the Y-12 Radiological Monitoring Plan (RMP), surface water is monitored at points that reflect individual facilities, as well as at points that reflect the combined contributions of all facilities. This monitoring plan does not consider other potential routes (i.e., airborne releases and food chains). Thus, a complete determination of total effective dose (TED) cannot be made based on this plan alone. The other routes from Y-12, and all routes from other DOE facilities on the Oak Ridge Reservation (e.g., Oak Ridge National Laboratory (ORNL) and The Heritage Center), must be considered in order to satisfy DOE Order 458.1 requirements. Determination of TED from all sites and pathways is done through the use of dose-assessment models and is documented in the Annual Site Environmental Report. This monitoring plan provides adequate monitoring goals for Y-12 surface water releases to provide input of sufficient sensitivity and accuracy to reliably determine the Y-12 surface water component of the TED. The routine radiological monitoring program is designed to monitor effluents at four types of locations: (1) treatment facilities, (2) other point and area source discharges, (3) instream locations, and (4) production building roof run-off. With this sampling and analysis program, data will be obtained on primary point sources as well as on locations that represent the composite of other potential sources. This plan will be reviewed periodically to determine necessary modifications to the sampling frequencies, parameters, and locations. Modifications, if any, will be based on the analysis of the previous data and its effectiveness in satisfying the objectives of this plan. Appendix A contains graphs of the sum of the DCS fractions for locations and frequencies contained in a previous version of this plan. The data was collected from January 2009 through December 2019. Each sample was analyzed, and each result was divided by the appropriate DCS to compute a DCS fraction. These fractions were summed for all isotopes. According to DOE –STD-1196-2011, the annual average of these sums should be below 1.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Resolved Resonance Region Analysis of 206 Pb, 207 Pb, and 208 Pb for Next Generation Lead-Cooled Fast Systems

Recently, great interest has been generated in using lead as a coolant for fast neutron systems and as a result it is important to investigate the ENDF/B-VIII.0 isotopic evaluations that comprise stable le ad. To this end, resonance parameters for 206 Pb, 207 Pb, and 208 Pb were re-evaluated because their resolved resonance regions extend beyond 0.5 MeV meaning resonance parameters used in reconstructing cross sections and elastic scattering angular distributions impact fast systems. The impact of resonance parameters is demonstrated by the differences between the evaluations in predicting experimental results from the fully modeled RPI Quasi-Differential Scattering Experiment via MCNPv6.2. In addition, MCNP KCODE calculations of lead-sensitive fast spectra critical benchmarks showed variations of keff on average of 400 pcm, caused solely from differences in elastic scattering angular distributions in 208 Pb. Re-evaluation entailed fitting data with the program SAMMY.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

Multiscale, mechanistic modeling of irradiation-enhanced silver diffusion in TRISO particles

Tristructural isotropic (TRISO) particles are under consideration for use in several proposed advanced nuclear reactor concepts. The silicon carbide (SiC) layer in TRISO acts as a barrier to prevent the release of the fission products. However, despite remarkable retention, silver (Ag) release has been observed from intact particles, which requires investigation since the Ag isotope ( 110m Ag) has a long half-life. Previous work focused on developing a multiscale, mechanistic model for Ag diffusion accounting for temperature and microstructure effect and has been successfully validated. In this work, we expand the previous model to account for irradiation-enhanced Ag diffusivity in SiC and improve its accuracy over a wider grain size and temperature ranges relevant for advanced reactor conditions. A temperature, grain size, and flux dependent diffusivity is therefore derived using the mesoscale code MARMOT and implemented in the fuel performance code BISON. The irradiation-enhanced Ag diffusivity in SiC is compared against experimental data and validated using BISON against Ag release measurements from the Advanced Gas Reactor Fuel Development and Qualification Program (AGR-1 and AGR-2). Herein, we quantify the impact of SiC grain size, irradiation, and temperature on Ag release. In agreement with previous studies, we find accounting for SiC grain size improves agreement between BISON predictions and experimental observations for most cases. In conclusion, we also find that accounting for irradiation improves agreement for cases where Ag release was underestimated, but the impact was less significant than accounting for microstructure.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2019

Geochemical characterization of floodplain sediments from Meander C and O in the East River Watershed, CO, USA

This data package is part of the Watershed Function SFA data collection and contains geochemical characterization of sediments as a function of depth in the pumphouse vicinity, including Meander C and Meander O (oxbow). This data was used in the manuscript "Fox, P.M., Bill, M., Heckman, K., Conrad, M., Anderson, C., Keiluweit, M., and Nico, P.S.Shale as a Source of Organic Carbon in Floodplain Sediments of a Mountainous Watershed" published in Journal of Geophysical Research: Biogeosciences. Data includes sieving, total organic carbon (TOC), total inorganic carbon (TIC), total nitrogen (TN), carbon isotopes (14C and 13C) of whole sediment. Sediment density fractionation data is also included, with measurements of TOC, TN, 14C and 13C on density fractions. Metal and carbon concentrations from various sediment extractions (HCl, dithionite, oxalate, water, and pyrophosphate) are included. Characterization of extracted carbon by fourier transform infrared spectroscopy (FTIR) and UV-Visible light spectroscopy. Characterization of density fractionated (light fractions) organic carbon by FTIR. Carbon X-ray spectroscopy (C near edge X-ray absorption fine structure spectroscopy [NEXAFS] and scanning transmission X-ray microscopy [STXM]) is also included for shale samples and sediment samples.Additional acknowledgements:1. M.K. and C.A. were supported by the Department of Energy, Office of Biological and Environmental Research, Subsurface Biosphere Research program (award no. DE-SC0016544).2. STXM and NEXAFS data was collected at the Canadian Light Source, which is supported by the Canada Foundation for Innovation, Natural Sciences and Engineering Research Council of Canada, the University of Saskatchewan, the Government of Saskatchewan, Western Economic Diversification Canada, the National Research Council Canada, and the Canadian Institutes of Health Research.3. Radiocarbon analysis was supported in part by the Radiocarbon Collaborative, which is jointly sponsored by the USDA Forest Service Northern Research Station, the KCCAMS Facility at UC Irvine, and Michigan Technological University.Update 11/06/2019: An .kml file was added with the GPS locations for all the sampling sites.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2018

The Neutron Macromolecular Crystallography Instruments at Oak Ridge National Laboratory: Advances, Challenges, and Opportunities

The IMAGINE and MaNDi instruments, located at Oak Ridge National Laboratory High Flux Isotope Reactor and Spallation Neutron Source, respectively, are powerful tools for determining the positions of hydrogen atoms in biological macromolecules and their ligands, orienting water molecules, and for differentiating chemical states in macromolecular structures. The possibility to model hydrogen and deuterium atoms in neutron structures arises from the strong interaction of neutrons with the nuclei of these isotopes. Positions can be unambiguously assigned from diffraction studies at the 1.5–2.5 Å resolutions, which are typical for protein crystals. Neutrons have the additional benefit for structural biology of not inducing radiation damage to protein crystals, which can be critical in the study of metalloproteins. Here we review the specifications of the IMAGINE and MaNDi beamlines and illustrate their complementarity. IMAGINE is suitable for crystals with unit cell edges up to 150 Å using a quasi-Laue technique, whereas MaNDi provides neutron crystallography resources for large unit cell samples with unit cell edges up to 300 Å using the time of flight (TOF) Laue technique. The microbial culture and crystal growth facilities which support the IMAGINE and MaNDi user programs are also described.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Chemical Compositions of Red Giant Stars from Habitable Zone Planet Finder Spectroscopy

We have used the Habitable Zone Planet Finder (HPF) to gather high-resolution, high signal-to-noise near-infrared spectra of 13 field red horizontal branch (RHB) stars, one open cluster giant, and one very metal-poor halo red giant. The HPF spectra cover the 0.81–1.28 μm wavelength range of the zyJ bands, partially filling the gap between the optical (0.4–1.0 μm) and infrared (1.5–2.4 μm) spectra already available for the program stars. We derive abundances of 17 species from LTE-based computations involving equivalent widths and spectrum syntheses, and estimate abundance corrections for the species that are most affected by departures from LTE in RHB stars. Generally good agreement is found between HPF-based metallicities and abundance ratios and those from the optical and infrared spectral regions. Light element transitions dominate the HPF spectra of these red giants, and HPF data can be used to derive abundances from species with poor or no representation in optical spectra (e.g., C i, P i, S i, K i). Attention is drawn to the HPF abundances in two field solar-metallicity RHB stars of special interest: one with an extreme carbon isotope ratio, and one with a rare, very large lithium content. The latter star is unique in our sample in exhibiting very strong He i 10830 Å absorption. The abundances of the open cluster giant concur with those derived from other wavelength regions. Detections of C i and S i in HD 122563 are reported, yielding the lowest metallicity determination of [S/Fe] from more than one multiplet.

47 OTHER INSTRUMENTATION↗

DOE OSTI2019

Elucidation of the Reaction Mechanism for High-Temperature Water Gas Shift over an Industrial-Type Copper–Chromium–Iron Oxide Catalyst

The water gas shift (WGS) reaction is of critical importance for the chemical industry, as it constitutes, coupled with methane reforming, the main industrial route to produce hydrogen. Copper–chromium–iron oxide-based catalysts have been widely used for the high-temperature WGS reaction industrially. The WGS reaction mechanism by the CuCrFeO x catalyst has been debated for years, mainly between a “redox” mechanism involving the participation of atomic oxygen from the catalyst and an “associative” mechanism proceeding via a surface formate-like intermediate. Here, advanced in situ characterization techniques (infrared spectroscopy, temperature-programmed surface reaction (TPSR), near-ambient pressure XPS (NAP-XPS), and inelastic neutron scattering (INS)) were applied to determine the nature of the catalyst surface and identify surface intermediate species under WGS reaction conditions. The surface of the CuCrFeO x catalyst is found to be dynamic and becomes partially reduced under WGS reaction conditions, forming metallic Cu nanoparticles on Fe 3 O 4 . Neither in situ IR not INS spectroscopy detect the presence of surface formate species during WGS. TPSR experiments demonstrate that the evolution of CO 2 and H 2 from the CO/H 2 O reactants follows different kinetics than the evolution of CO 2 and H 2 from HCOOH decomposition (molecule mimicking the associative mechanism). Steady-state isotopic transient kinetic analysis (SSITKA) (CO + H 2 16 O → CO + H 2 18 O) exhibited significant 16 O/ 18 O scrambling, characteristic of a redox mechanism. Computed activation energies for elementary steps for the redox and associative mechanism by density functional theory (DFT) simulations indicate that the redox mechanism is favored over the associative mechanism. The combined spectroscopic, computational, and kinetic evidence in the present study finally resolves the WGS reaction mechanism on the industrial-type high-temperature CuCrFeO x catalyst that is shown to proceed via the redox mechanism.

SSITKA↗