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At least 1,729 records · Page 96

Effects of redox cycling of iron in nontronite on reduction of technetium

In situ technetium-99 ( 99 Tc) immobilization by Fe(II) associated with clay minerals is a potential cost-effective method for Tc remediation at contaminated sites. The oxidation state of Fe is constantly cycled in sedimentary environments, however the effect of this cycle on Tc reduction and immobilization has not yet been investigated. The objective of this project was therefore to study how multiple cycles of reduction-reoxidation of Fe-rich clay mineral, nontronite, affected its reactivity toward Tc (VII) reduction. Iron-rich nontronite NAu-2 was used as a model clay mineral. NAu-2 suspension was first bioreduced by Shewanella putrefaciens CN32, which was subsequently re-oxidized by air. Three cycles of reduction-oxidation were conducted and bioreduced NAu-2 samples from all three cycles were collected and used for Tc(VII) reduction experiments. Each redox cycle resulted in a small fraction of dissolution of small size and/or poorly crystalline NAu-2. The released Fe(II) from the dissolution was likely adsorbed onto NAu-2 surface/edge sites with a high reactivity. Upon exposure to O2, this reactive Fe(II) fraction was oxidized more rapidly than structural Fe(II) and may have accounted for a two-step reoxidation kinetics of NAu-2 associated Fe(II): rapid oxidation over first few hours followed by slow oxidation. Progressive increase of this reactive fraction of Fe(II), from increased dissolution, accounted for the successively higher rate of bioreduction and reoxidation with increased redox cycles. The same Fe redistribution accounted for two-step Tc(VII) reduction kinetics as well. Rapid Tc(VII) reduction in the first few hours may be attributed to a small fraction of highly reactive Fe(II) at the NAu-2 surface/edge sites, and more steady Tc(VII) reduction over longer time may be carried out by structural Fe(II). Similar to the increased rates of Fe(III) reduction and Fe(II) oxidation, the Tc(VII) reduction rate also increased with redox cycles and could be explained by progressive increase of the reactive Fe(II) on NAu-2 surface/edges. Iron-rich clay minerals undergo important changes after redox cycles, but eventually reach a steady state with continued reactivity toward heavy metals.

36 MATERIALS SCIENCE↗

Sputtered indium tin oxide as a recombination layer formed on the tunnel oxide/poly-Si passivating contact enabling the potential of efficient monolithic perovskite/Si tandem solar cells

We focus on utilizing sputtered indium tin oxide (ITO) as a recombination layer, having low junction damage to an n-type silicon solar cell with a front-side tunnel oxide passivating electron contact, thereby enabling the development of a high efficiency monolithic perovskite/Si tandem device. High transparency and low resistivity ITO films are deposited via low power DC magnetron sputtering at room temperature onto a front-side thin SiO x /n + poly-Si contact in a complete Cz n-Si cell with a back-side Al 2 O 3 /SiN x passivating boron-diffused p + -emitter on a random pyramid textured surface. We report the cell characteristics before and after ITO sputtering, and we find a cure at 250 °C in air is highly effective at mitigating any sputtering induced damage. Our ITO coated sample resulted in an implied open-circuit voltage (iV oc ) of 684.7 ± 11.3 mV with the total saturation current density of 49.2 ± 14.8 fA/cm 2 , an implied fill factor (iFF) of 81.9 ± 0.8%, and a contact resistivity in the range of 60 mΩ-cm 2 to 90 mΩ-cm 2 . After formation of a local Ag contact to the rear emitter and sputtered ITO film as the front-side contact without grid fingers, the pseudo-efficiency of 20.2 ± 0.5% was obtained with the V oc of 670.4 ± 7 mV and pseudo FF of 77.3 ± 1.3% under simulated one sun with the calculated short-circuit current density of 30.9 mA/cm 2 from the measured external quantum efficiency. Furthermore, our modelling result shows that efficiency exceeding 25% under one sun is practically achievable in perovskite/Si tandem configuration using the ITO recombination layer connecting a perovskite top cell and a poly-Si bottom cell.

14 SOLAR ENERGY↗

Direct Air Capture and Sequestration of CO 2 by Accelerated Indirect Aqueous Mineral Carbonation under Ambient Conditions

Mineralization of gaseous carbon dioxide into solid carbonates using alkaline industrial residues such as coal fly ash has a dual advantage of reducing the carbon dioxide footprint of coal power plants and improving ash utilization. However, the slow mineral carbonation rate under atmospheric conditions is a major challenge, especially when using natural minerals or industrial residues for direct air capture (DAC) of CO 2 . In this study, using coal fly ash samples and concentrated alkali carbonate aqueous solutions as a recyclable solvent, we show the feasibility of coupling mineral carbonation with DAC under atmospheric conditions. Findings show that carbonation efficiency is best under alkaline conditions, achieving as high as ~80% conversion to calcium carbonates within 1 h in a 1.9 M sodium carbonate solution. Based on the experimental results, a process coupling DAC and mineral carbonation that operates entirely under ambient conditions is proposed. Here, the techno-economic and life cycle assessments for the proposed process project a levelized cost of $\$116$–133/t-CO 2 -sequestered (US $\$2019$) and process carbon emissions (GWP) in the range of 0.03–0.25 t-CO 2 e/t-CO 2 -sequestered. Considering the low cost, simplicity, and gigaton-scale sequestration potential, we believe that DAC based on alkaline industrial residue carbonation can be considered a “low-hanging fruit” in the pursuit of negative emissions to combat climate change.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Solvent- and catalyst-free mechanochemical synthesis of alkali metal monohydrides

Alkali metal monohydrides, AH (A = Li–Cs) have been synthesized in quantitative yields at room temperature by reactive milling of alkali metals in the presence of hydrogen gas at 200 bar or less. The mechanochemical approach reported here eliminates problems associated with the malleability of alkali metals — especially Li, Na, and K — and promotes effective solid–gas reactions, ensuring their completion. This is achieved by incorporating a certain volume fraction of the corresponding hydride powder as a process control agent, which allows continuous and efficient milling primarily by coating the surface of metal particles, effectively blocking cold welding. Formation of high-purity crystalline monohydrides has been confirmed by powder X-ray diffraction, solid-state NMR spectroscopy, and volumetric analyses of reactively desorbed H 2 from as-milled samples. The proposed synthesis method is scalable and particularly effective for extremely air-sensitive materials, such as alkali and alkaline earth metal hydrides. Furthermore, the technique may also be favorable for production in continuous reactors operating at room temperature, thereby reducing the total processing time, energy consumption and, hence, the cost of production of these hydrides or their derivatives and composites.

36 MATERIALS SCIENCE↗

Post-growth annealing induced change of conductivity in As-doped ZnO grown by radio frequency magnetron sputtering

Arsenic-doped ZnO films were fabricated by radio frequency magnetron sputtering method at a relatively low substrate temperature of 200 deg. C. Post-growth annealing in air was carried out up to a temperature of 1000 deg. C. The samples were characterized by Hall measurement, positron annihilation spectroscopy (PAS), secondary ion mass spectroscopy (SIMS), and cathodoluminescence (CL). The as-grown sample was of n-type and it converted to p-type material after the 400 deg. C annealing. The resulting hole concentration was found to increase with annealing temperature and reached a maximum of 6 x 10{sup 17} cm{sup -3} at the annealing temperature of 600 deg. C. The origin of the p-type conductivity was consistent with the As{sub Zn}(V{sub Zn}){sub 2} shallow acceptor model. Further increasing the annealing temperature would decrease the hole concentration of the samples finally converted the sample back to n-type. With evidence, it was suggested that the removal of the p-type conductivity was due to the dissociation of the As{sub Zn}(V{sub Zn}){sub 2} acceptor and the creation of the deep level defect giving rise to the green luminescence.

36 MATERIALS SCIENCE↗

Lithium-loaded liquid scintillator production for the PROSPECT experiment

This work reports here the production and characterization of lithium-loaded liquid scintillator (LiLS) for the Precision Reactor Oscillation and Spectrum Experiment (PROSPECT) . Fifty-nine 90 liter batches of LiLS ( 6 Li mass fraction 0.082%±0.001%) were produced and samples from all batches were characterized by measuring their optical absorbance relative to air, light yield relative to a pure liquid scintillator reference, and pulse shape discrimination capability. Fifty-seven batches passed the quality assurance criteria and were used for the PROSPECT experiment.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Extraction of the muon signals recorded with the surface detector of the Pierre Auger Observatory using recurrent neural networks

The Pierre Auger Observatory, at present the largest cosmic-ray observatory ever built, is instrumented with a ground array of 1600 water-Cherenkov detectors, known as the Surface Detector (SD). The SD samples the secondary particle content (mostly photons, electrons, positrons and muons) of extensive air showers initiated by cosmic rays with energies ranging from 1017eV up to more than 1020eV. Measuring the independent contribution of the muon component to the total registered signal is crucial to enhance the capability of the Observatory to estimate the mass of the cosmic rays on an event-by-event basis. However, with the current design of the SD, it is difficult to straightforwardly separate the contributions of muons to the SD time traces from those of photons, electrons and positrons. In this paper, we present a method aimed at extracting the muon component of the time traces registered with each individual detector of the SD using Recurrent Neural Networks. We derive the performances of the method by training the neural network on simulations, in which the muon and the electromagnetic components of the traces are known. We conclude this work showing the performance of this method on experimental data of the Pierre Auger Observatory. We find that our predictions agree with the parameterizations obtained by the AGASA collaboration to describe the lateral distributions of the electromagnetic and muonic components of extensive air showers.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Risk reporting in the Chinese news media in response to radiation threat from the Fukushima nuclear reactor crisis

On March 11, 2011, the northeastern coast of Japan was struck by 9.0-magnitude earthquake that triggered a devastating tsunami. Aside from the huge toll in people's lives and severe damages to property, the tremor sent the Fukushima Daiichi Nuclear Power Plant on a tailspin, causing hydrogen explosions in three reactors, and sending radioactive materials into the air and bodies of water. Declared the largest nuclear disaster since Chernobyl, the crisis threatened neighboring countries, including China (International Business Times, 2011). On March 28, low levels of iodine-131, cesium-137 and strontium, believed to have drifted from Japan, were detected in the air over Heilongjiang province in the northeast part of China and in seawater samples collected in the eastern coastal areas (Qianjiang Eve News, 2011). Because these chemicals can enter the food chain and adversely affect human health (Ifeng.com, 2011), people became understandably anxious and the government had to avert panic. This study asks: How did the Chinese media report the risks attendant to this event? A content analysis of 45 straight news reports published by the Chinese press from March 16, 2011 to April 25, 2011 was conducted. The analysis focused on how the media explained the risk, portrayed potential harm, reported on government actions to safeguard public health, and provided suggestions to reduce public fear. The sources of information cited in the reports were also identified. The articles examined were collected from People.com, a comprehensive online archive of news reports, using 'Fukushima' and 'nuclear radiation' as search terms. The results indicated journalistic practices that left much to be desired in terms of risk reporting. First, the articles explained little about the technical aspects of the radiation leaks and failed to give audiences a general indication of levels of risk. Second, the media over-emphasized the government's position that the environment was safe despite the more rampant word-of-mouth reports to the contrary, a slant that may have done nothing to allay public fear. Third, there was a dearth of information about what the government intends to do to alleviate the situation and suggestions about what people can do to protect themselves. The themes of news reports may be attributed to experts from research institutions and government officials who were the most frequently cited sources of facts, analyses, interpretations, and opinions. Scientists and nuclear experts were cited the most in the news reports. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Samarium electrodeposited acetate and oxide thin films on stainless steel substrate characterized by XPS

Characterization of a samarium thin film deposited on a stainless steel substrate using molecular electrodeposition was carried out using a Thermo Scientific K-Alpha X-ray photoelectron spectrometer. We studied two types of samarium electrodeposition samples, one as-deposited and one heated to 700 °C in an air flow. Survey scans include peaks coming from the stainless steel substrate, such as Fe and Cr. An X-ray photoelectron spectroscopy (XPS) survey spectrum, Sm 3d, C 1s, and O 1s narrow scans are shown. It was determined that the heating process decomposed the deposited Sm acetate to Sm 2 O 3 using XPS.

36 MATERIALS SCIENCE↗

Material Testing of Coated Alloys in a Syngas Combustion Environment Year 6 - Activity 1.13 - Development of a National Center for Hydrogen Technology

Modifications were made to the inlet of the existing Energy & Environmental Research Center (EERC) thermal oxidizer to accommodate side-by-side coupon holders for exposure testing. Two 5-day tests with over 200 hours of total exposure time were completed. The first week of testing was conducted in enriched air-blown mode, with coupon temperatures ranging from 128° to 272°F. Carbonyl sampling was conducted, but it was discovered after the fact that the methodology used was producing very low recoveries of iron and nickel carbonyl. Therefore, the data generated during this week of testing were not considered accurate. The second week of testing was conducted in oxygen-blown mode, with coupon temperatures ranging from 220° to 265°F. Two improved methods were used to measure carbonyl concentration during this week of testing. These methods produced results closer to equilibrium calculations. Since both weeks of testing mostly produced a product gas with approximately 15%–18% carbon monoxide, it was felt that actual carbonyl concentrations for Week 1 should be very similar to those measured during Week 2. The revised carbonyl sampling methodology used during the second week of testing greatly improved the recovery of iron and nickel carbonyl in the sample. Even though the sampling results obtained from the first week were inaccurate, the results from the second week can be used as an estimate for the periods during which the gasifier was operating under similar conditions and producing similar product gas compositions. Specifically, Test Periods 2 and 3 from the first week were similar to the conditions run during the second week. For a product gas containing roughly 15%–18% CO and a coupon temperature of approximately 220°–270°F, the nickel carbonyl concentration should be about 0.05–0.1 ppm and the iron carbonyl concentration should be about 0.1–0.4 ppm. After each week of testing the coupons were recovered from the coupon holder, weighed, and shipped back to Siemens for analysis.

42 ENGINEERING↗

Final Progress Report for Collaborative Research: Aging of Black Carbon during Atmospheric Transport: Understanding Results from the DOE’s 2010 CARES and 2012 ClearfLo Campaigns

Over the course of this project, we have analyzed data and samples from the Carbonaceous Aerosol and Radiative Effects Study (CARES) and the Clear air for London (ClearfLo) campaign, as well as conducted or participated in laboratory experiments designed to better understand black carbon mixing state and climate-relevant properties. The laboratory campaigns took place at the Pacific Northwest National Laboratory and Carnegie Mellon University to study various climate-relevant aerosol properties of different sources of soot mixing with secondary organic aerosol precursors. Results from some of these activities were summarized in the previous progress report. This final report presents the manuscripts that have been published (many in the period since the last progress report), lists presentations at different conferences based on grant-related activities, and presents some results that are likely to be submitted for publication in the near future.

54 ENVIRONMENTAL SCIENCES↗

Measurement of radiolytic hydrogen generation and impact of drying treatments on reactor exposed and surrogate aluminum materials

Technical challenges associated with dry storage of Aluminum-clad Spent Nuclear Fuel (ASNF) include a need to better understand the potential extent of gaseous molecular hydrogen (H 2 ) production through radiolytic degradation of the aluminum (oxy)hydroxide films present on ASNF. The characterization of radiolytic gas generation from ASNF (oxy)hydroxide layers has been identified as a key knowledge gap which poses a technical challenge to the long-term storage of ASNF. Task 2 of the action plan for the extended (>50 years) dry storage of ASNF addresses this gap. Previous radiolysis studies performed under Task 2 established baseline estimates of H 2 generation rates from the attendant hydrated oxides. The results confirmed that net radiolytic H 2 production has a dependency on absorbed gamma dose, as well as relative humidity and cover gas composition (air, nitrogen, and argon). Further experiments revealed that the physisorbed water on the samples may significantly impact the radiolytic H 2 yield. This phenomenon complicates the determination of H 2 generation rates for hydrated oxides, which may lead to inaccurate modeling predictions of the long-term H 2 yields in sealed storage systems containing ASNF, particularly when compared to spent fuel casks which have undergone some drying process intended to remove physically- and chemically-bound water. This report describes the testing methods utilized and the hydrogen generation results obtained in an investigation of the effects of gamma irradiation on aluminum materials for a variety of (oxy)hydroxide surface compositions and drying conditions. The testing methods included small-area aluminum material testing in ampules, and large-area aluminum material testing in steel vessels. Test material preparation, irradiation, and radiolytic H 2 measurement methods are summarized. The measured H 2 concentrations, which reflect the variable initial hydrated inventory and drying treatments, are compared to one another as well as to previously published data, to identify the primary factors affecting radiolytic H 2 generation rates and potential equilibrium H 2 concentrations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Los Alamos National Laboratory 2022 Annual Site Environmental Report (Rev. 2)

Los Alamos National Laboratory (Laboratory) annual site environmental reports are prepared each year by the Laboratory’s environmental organizations as required by U.S. Department of Energy Order 231.1B, Administrative Change 1, Environment, Safety, and Health Reporting, and Order 458.1, Administrative Change 4, Radiation Protection of the Public and the Environment. The chapters in this report discuss our compliance with environmental laws, regulations, and orders (Chapter 2, Compliance Summary); how we manage the Laboratory’s environmental performance and assure the quality of data from analysis of environmental samples (Chapter 3, Environmental Programs and Analytical Data Quality); how we monitor for air emissions of radioactive materials and for weather conditions (Chapter 4, Air Quality); how we monitor for effects of Laboratory operations on groundwater quality (Chapter 5, Groundwater Protection); how we monitor the levels of chemicals and radionuclides in storm water runoff and sediment (Chapter 6, Watershed Quality); how we monitor for the levels and effects of chemicals and radionuclides in plants, animals, soil, and vegetation (Chapter 7, Ecosystem Health); and finally, what radioactive dose or risk from chemical exposure that members of the public could experience as a result of Laboratory operations (Chapter 8, Public Dose and Risk Assessment).

54 ENVIRONMENTAL SCIENCES↗

Isothermal and cyclic oxidation at 1000 and 1100 deg C of four nickel-base alloys: NASA-TRW VIA, B-1900, 713C, and 738X

The isothermal and cyclic oxidation resistance of four cast Ni-base gamma + gamma prime alloys, NASA-TRW Via, B-1900, 713C, and 738X, was determined in still air at 1000 and 1100 C. The oxidation process was evaluated by specific sample weight change with time, sample thickness change, X-ray diffraction of the scales, and sample metallography. The behavior is discussed in terms of the Cr, Al, and refractory metal contents of the alloys.

Barrett, C. A.↗

Balloon-borne photoionization mass spectrometer for measurement of stratospheric gases

A balloon-borne photoionization mass spectrometer used to measure stratospheric trace gases is described. Ions are created with photons from high-intensity krypton discharge lamps and a quadrupole mass analyzer is employed for ion identification. Differential pumping is achieved with liquid helium cryopumping. To insure measurement of unperturbed stratospheric air, the entire system is contained in a sealed gondola and the atmospheric sample is taken some distance away during descent. The photoionization technique allows the detection of a low ionization potential constituent, such as nitric oxide, at less than a part in one billion in the presence of the major atmospheric gases and their isotopes. Operation of the mass spectrometer system was demonstrated during a daytime flight from Palestine, Texas on 26 April 1977. The sensitivity achieved and the unique selectivity afforded by this technique offer a capability for trace constituent measurement not possible with the more conventional electron impact ionization approach.

Aikin, A. C.↗

Assessment of potential exposure to friable insulation materials containing asbestos

Asbestos and the procedures for assessing potential exposure hazards are discussed. Assessment includes testing a bulk sample of the suspected material for the presence of asbestos, and monitoring the air, if necessary. Based on field inspections and laboratory analyses, the health hazard is evaluated, and abatement measures are taken if a potential hazard exists. Throughout the assessment and abatement program, all applicable regulations are administered as specified by the Environmental Protection Agency and the Occupational Safety and Health Administration.

Kim, W. S.↗

Enhanced capabilities and updated users manual for axial-flow turbine preliminary sizing code TURBAN

Several modifications have been made to the axial-flow turbine preliminary sizing code TURBAN. Turbine cooling has been added to the analysis. New alternative input options allow direct specification of stage reaction, stage work factor, and stage work split. The Reynolds number loss dependency was modified and an internal calculation of air viscosity was added. A complete description of input and output along with sample cases are included.

Glassman, Arthur J.↗

High Temperature Degradation Mechanisms in Polymer Matrix Composites

Polymer matrix composites are increasingly used in demanding structural applications in which they may be exposed to harsh environments. The durability of such materials is a major concern, potentially limiting both the integrity of the structures and their useful lifetimes. The goal of the current investigation is to develop a mechanism-based model of the chemical degradation which occurs, such that given the external chemical environment and temperatures throughout the laminate, laminate geometry, and ply and/or constituent material properties, we can calculate the concentration of diffusing substances and extent of chemical degradation as functions of time and position throughout the laminate. This objective is met through the development and use of analytical models, coupled to an analysis-driven experimental program which offers both quantitative and qualitative information on the degradation mechanism. Preliminary analyses using a coupled diffusion/reaction model are used to gain insight into the physics of the degradation mechanisms and to identify crucial material parameters. An experimental program is defined based on the results of the preliminary analysis which allows the determination of the necessary material coefficients. Thermogravimetric analyses are carried out in nitrogen, air, and oxygen to provide quantitative information on thermal and oxidative reactions. Powdered samples are used to eliminate diffusion effects. Tests in both inert and oxidative environments allow the separation of thermal and oxidative contributions to specimen mass loss. The concentration dependency of the oxidative reactions is determined from the tests in pure oxygen. Short term isothermal tests at different temperatures are carried out on neat resin and unidirectional macroscopic specimens to identify diffusion effects. Mass loss, specimen shrinkage, the formation of degraded surface layers and surface cracking are recorded as functions of exposure time. Geometry effects in the neat resin, and anisotropic diffusion effects in the composites, are identified through the use of specimens with different aspect ratios. The data is used with the model to determine reaction coefficients and effective diffusion coefficients. The empirical and analytical correlations confirm the preliminary model results which suggest that mass loss at lower temperatures is dominated by oxidative reactions and that these reaction are limited by diffusion of oxygen from the surface. The mechanism-based model is able to successfully capture the basic physics of the degradation phenomena under a wide range of test conditions. The analysis-based test design is successful in separating out oxidative, thermal, and diffusion effects to allow the determination of material coefficients. This success confirms the basic picture of the process; however, a more complete understanding of some aspects of the physics are required before truly predictive capability can be achieved.

Cunningham, Ronan A.↗