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DOE OSTI2016

Characterization and Recovery of Rare Earths from Coal and By-Products

Coal is a precious resource, both in the United States and around the world. The United States has a 250-year supply of coal, and generates between 30 - 40% of its electricity through coal combustion. Approximately 1 Gt of coal has been mined annually in the US, although the 2015 total will likely be closer to 900 Mt (http://www.eia.gov/coal/production/quarterly/). Most of the coal is burned for power generation, but substantial quantities are also employed in the manufacture of steel, chemicals, and activated carbons. Coal has a positive impact upon many industries, including mining, power, rail transportation, manufacturing, chemical, steel, activated carbon, and fuels. Everything that is in the earth’s crust is also present within coal to some extent, and the challenge is always to utilize abundant domestic coal in clean and environmentally friendly manners. In the case of the rare earths, these valuable and extraordinarily useful elements are present within the abundant coal and coal by-products produced domestically and world-wide. These materials include the coals, as well as the combustion by-products such as ashes, coal preparation wastes, gasification slags, and mining by-products. All of these materials can be viewed as potential sources of rare earth elements. Most of the common inorganic lanthanide compounds, such as the phosphates found in coal, have very high melting, boiling, and thermal decomposition temperatures, allowing them to concentrate in combustion and gasification by-products. Furthermore, rare earths have been found in interesting concentrations in the strata above and below certain coal seams. Much of the recent research on coal utilization in the United States has focused upon the capture of pollutants such as acid gases, particulates, and mercury, and the greenhouse gas carbon dioxide. The possible recovery of rare earth and other critical elements from abundant coal and by-products is an exciting new research area, representing a dramatic paradigm shift for coal.

01 COAL, LIGNITE, AND PEAT↗

DOE OSTI2025

MARIE: A Python-Based Framework for Comprehensive Fuel Recycling Modeling

One of the most pressing challenges to the continued deployment of nuclear energy systems is in the ultimate management and disposition of discharged fuel assemblies. While reprocessing and recovery of valuable materials from UNF assemblies has been considered as part of an overall strategy for minimization of the volume of reactor-based wastes to be managed, the deployment of commercial-scale reprocessing facilities presents an enormous economic challenge. The MARIE software package has been developed as a means of confronting this challenge. Representing components of a generic fuel reprocessing operation as individual physical processes, MARIE is designed as a modular framework intended to allow for analysis and cost-optimization for a hypothetical reprocessing facility while realistically accounting for the physical characteristics of the used fuel source term, such as decay heat, activity, and radiation dose (informing corresponding shielding requirements). Capabilities supported by MARIE include head-end operations such as fuel shearing, voloxidation, and dissolution; generic solvent extraction operations informed by available open-literature data; a suite of unit operations intended to represent electrochemical processing of used fuel assemblies (i.e., oxide reduction, electrorefining, and electrowinning); and finally, accounting for both costs and physical features of discharged waste streams, which can be used to inform follow-on analyses such as the feasibility of deep-borehole disposal of HLW. This paper presents an overview of the MARIE software capabilities, including how individual unit operations are implemented to enable a larger-scale optimization of a hypothetical reprocessing operation on aspects such as cost and recovery of valuable materials.

Skutnik, Steve [ORNL] (ORCID:000000016441135X)↗

DOE OSTI2021

An Artificial Neural Network System for Photon-Based Active Interrogation Applications

Active interrogation (AI) is a promising technique to detect shielded special nuclear materials (SNMs). At the University of Michigan, we are developing a photon-based AI system that uses bremsstrahlung radiation from an electron linear accelerator (linac) as an ionizing source and stilbene organic scintillating detectors for neutron detection. Stilbene scintillators are sensitive to fast neutrons and photons and have excellent pulse shape discrimination (PSD) capabilities. The traditional charge integration (CI) method commonly used for PSD analysis eliminates piled-up pulses and relies on a particle discrimination line to separate neutrons and photons. The presence of the intense photon flux during AI creates a significant number of piled-up events in the stilbene scintillator, thereby posing a great challenge to the traditional CI method. Identifying true single neutron pulses becomes challenging due to the presence of a pile-up cloud and overlapping neutron, photon and pile-up clouds in the PSD analysis. To mitigate the effect of pulse pile up and identify true single neutron pulses from stilbene scintillators, an artificial neural network (ANN) system is developed. The developed ANN system identifies single neutron pulses and neutron-photon combinations from piled-up events. The results obtained from a 252Cf measurement in the presence of the intense photon flux show that the developed ANN system outperforms the traditional CI method. Since many piled-up events lie above the particle discrimination line, they get misclassified as neutrons by the traditional CI method resulting in 25% overestimation of the net neutron count rate during the linac pulse. The overall net neutron count rate (single and restored neutrons) during the linac pulse, estimated by the ANN system is 60% of the ground truth. Energy spectroscopy of the ANN attributed single neutron pulses further provides evidence on the detection of prompt fission neutrons from the 252Cf fission source.

42 ENGINEERING↗

DOE OSTI2015

Adsorbent Alkali Conditioning for Uranium Adsorption from Seawater. Adsorbent Performance and Technology Cost Evaluation

The Fuel Resources program of the Fuel Cycle Research and Development program of the Office of Nuclear Energy (NE) is focused on identifying and implementing actions to assure that nuclear fuel resources are available in the United States. An immense source of uranium is seawater, which contains an estimated amount of 4.5 billion tonnes of dissolved uranium. This unconventional resource can provide a price cap and ensure centuries of uranium supply for future nuclear energy production. NE initiated a multidisciplinary program with participants from national laboratories, universities, and research institutes to enable technical breakthroughs related to uranium recovery from seawater. The goal is to develop advanced adsorbents to reduce the seawater uranium recovery technology cost and uncertainties. Under this program, Oak Ridge National Laboratory (ORNL) has developed a new amidoxime-based adsorbent of high surface area, which tripled the uranium capacity of leading Japanese adsorbents. Parallel efforts have been focused on the optimization of the physicochemical and operating parameters used during the preparation of the adsorbent for deployment. A set of parameters that need to be optimized are related to the conditioning of the adsorbent with alkali solution, which is necessary prior to adsorbent deployment. Previous work indicated that alkali-conditioning parameters significantly affect the adsorbent performance. Initiated in 2014, this study had as a goal to determine optimal parameters such as base type and concentration, temperature, and duration of conditioning that maximize the uranium adsorption performance of amidoxime functionalized adsorbent, while keeping the cost of uranium production low. After base-treatment at various conditions, samples of adsorbent developed at ORNL were tested in this study with batch simulated seawater solution of 8-ppm uranium concentration, batch seawater spiked with uranium nitrate at 75-100 ppb uranium, and continuous-flow natural seawater at the Pacific Northwest National Laboratory (PNNL). Fourier Transform Infrared (FTIR) spectroscopy, Nuclear Magnetic Resonance (NMR) spectroscopy, Scanning Electron Microscopy (SEM), and elemental analysis were used to characterize the adsorbent at different stages of adsorbent preparation and treatment. The study can be divided into two parts: (A) investigation of optimal parameters for KOH adsorbent conditioning and (B) investigation of other possible agents for alkali conditioning, including cost analysis on the basis of uranium production. In the first part of the study, tests with simulated seawater containing 8 ppm uranium showed that the uranium adsorption capacity increased with an increase in the KOH concentration and conditioning time and temperature at each of the KOH concentrations used. FTIR and solid state NMR studies indicated that KOH conditioning converts the amidoxime functional groups into more hydrophilic carboxylate. The longer the KOH conditioning time, up to three hours, the higher was the loading capacity from the simulated seawater solution which is composed of only uranyl, sodium, chloride, and carbonate ions. Marine testing with natural seawater, on the other hand, showed that the uranium adsorption capacity of the adsorbent increased with KOH conditioning temperature, and gradually decreased with increasing KOH conditioning time from one hour to three hours at 80 C. This behavior is due to the conversion of amidoxime to carboxylate. The carboxylate groups are needed to increase the hydrophilicity of the adsorbent; however, conversion of a significant amount of amidoxime to carboxylate leads to loss in selectivity toward uranyl ions. Thus, there is an optimum KOH conditioning time for each temperature at which an optimum ratio between amidoxime and carboxylate is reached. For the case of base conditioning with 0.44 M KOH at 80 C, the optimal conditioning time is 1 hour, with respect to the highest uranium loading capacity from natural seawater. Uptake of other metal ions such as V, Fe, and Cu follows the same trend as that of uranium. Also, the uptake of Ca, Mg, and Zn ions increased with increasing KOH conditioning time, probably due to formation of more carboxylates, which leads to conversion of uranium-selective binding sites to less selective sites. In the second part of the study, inorganic based reagents such as sodium hydroxide (NaOH), sodium carbonate (Na 2 CO 3 ), cesium hydroxide (CsOH), as well as organic based reagents such as ammonium hydroxide (AOH), tetramethylammonium hydroxide (TMAOH), tetraethylammonium hydroxide (TEAOH), triethylmethylammonium hydroxide (TEMAOH), tetrapropylammonium hydroxide (TPAOH) and tetrabutylammonium hydroxide (TBAOH), in addition to KOH, were used for alkaline conditioning. NaOH has emerged as a better reagent for alkaline conditioning of amidoxime-based adsorbent because of higher uranium uptake capacity, higher uranium uptake selectivity ...

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2021

Report on Mowry Shale Thermal Maturity Mapping in the Powder River Basin, Wyoming

The Enhanced Oil Recovery Institute (EORI) has completed a map of thermal maturity of the Mowry Shale in the Powder River Basin (PRB). Thermal maturity, the degree to which the total organic carbon in a formation has been transformed from kerogen to producible hydrocarbons due to heat and pressure, is an important measure for not just the quality of a source rock, but also helps for delineating areas more favorable for unconventional drilling. There is a dearth of published Mowry maturity maps available for the PRB and this publication endeavors to provide a detailed map based on a large, public data set covering the Wyoming portion of the PRB. Additional data, currently held confidential by operators in the basin, would be of benefit to future iterations of this map.

02 PETROLEUM↗

DOE OSTI2020

CO 2 Injection Monitoring with a Scalable, Automated Sparse Seismic Array

Conference presentation at American Institute of Chemical Engineers (AIChE) Annual Meeting, Virtual, November 16–20, 2020. The scalable, automated sparse seismic array (SASSA) method has been ideated as a cost-effective alternative or complementary to conventional 3D seismic methods. Based on a sparse array of receivers deployed strategically on Earth’s surface and one or more fixed seismic sources, the SASSA method can be used to study specific portions of the subsurface to detect the movement of CO 2 in a reservoir with lower environmental footprint and shorter turnaround time to deliver results than conventional 3D seismic methods. Energy & Environmental Research Center (EERC) carried out seismic monitoring of an oilfield undergoing CO 2 enhanced oil recovery in Montana, USA, using the SASSA method.

02 PETROLEUM↗

NASA NTRS2003

Applying Model-Based Reasoning to the FDIR of the Command and Data Handling Subsystem of the International Space Station

All of the International Space Station (ISS) systems which require computer control depend upon the hardware and software of the Command and Data Handling System (C&DH) system, currently a network of over 30 386-class computers called Multiplexor/Dimultiplexors (MDMs)[18]. The Caution and Warning System (C&W)[7], a set of software tasks that runs on the MDMs, is responsible for detecting, classifying, and reporting errors in all ISS subsystems including the C&DH. Fault Detection, Isolation and Recovery (FDIR) of these errors is typically handled with a combination of automatic and human effort. We are developing an Advanced Diagnostic System (ADS) to augment the C&W system with decision support tools to aid in root cause analysis as well as resolve differing human and machine C&DH state estimates. These tools which draw from sources in model-based reasoning[ 16,291, will improve the speed and accuracy of flight controllers by reducing the uncertainty in C&DH state estimation, allowing for a more complete assessment of risk. We have run tests with ISS telemetry and focus on those C&W events which relate to the C&DH system itself. This paper describes our initial results and subsequent plans.

Robinson, Peter↗

DOE OSTI2021

Report on Mowry Shale Thermal Maturity Mapping in the Powder River Basin, Wyoming

58 GEOSCIENCES↗

DOE OSTI2017

Seed origin and warming constrain lodgepole pine recruitment, slowing the pace of population range shifts

Understanding how climate warming will affect the demographic rates of different ecotypes is critical to predicting shifts in species distributions. In this study, we present results from a common garden, climate change experiment in which we measured seedling recruitment of lodgepole pine, a widespread North American conifer that is also planted globally. Seeds from a low-elevation provenance had more than three-fold greater recruitment to their third year than seeds from a high-elevation provenance across sites within and above its native elevation range and across climate manipulations. Heating halved recruitment to the third year of both low- and high-elevation seed sources across the elevation gradient, while watering more than doubled recruitment, alleviating some of the negative effects of heating. Demographic models based on recruitment data from the climate manipulations and long-term observations of adult populations revealed that heating could effectively halt modeled upslope range expansion except when combined with watering. Simulating fire and rapid postfire forest recovery at lower elevations accelerated lodgepole pine expansion into the alpine, but did not alter final abundance rankings among climate scenarios. Regardless of climate scenario, greater recruitment of low-elevation seeds compensated for longer dispersal distances to treeline, assuming colonization was allowed to proceed over multiple centuries. In conclusion, our results show that ecotypes from lower elevations within a species’ range could enhance recruitment and facilitate upslope range shifts with climate change.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2016

TU-H-CAMPUS-TeP2-02: FLASH Irradiation Improves the Therapeutic Index Following GI Tract Irradiation

Purpose: To investigate and characterize the radiobiological effectiveness of very high dose rate radiotherapy (FLASH) compared to conventional irradiation in an in vivo model. Methods: The gastrointestinal (GI) tract of C57BL/6 mice were irradiated with doses ranging between 10 and 18 Gy using a custom stereotactic jig. A Varian Clinac 21EX was modified to allow dose rates ranging from 0.05 to 240 Gy/s at the position of the mirror. With the gantry at 180 degrees, the jig holding the individual animals was placed above the mirror to take advantage of the reduced source to target distance. Mice were irradiated with 20MeV electrons. Following irradiation, the mice were monitored twice daily for morbidity and daily for weight changes. Results: Mice irradiated with FLASH irradiation had lower weight loss compared to the mice receiving conventional irradiation. Following FLASH irradiation, a maximum weight loss of ∼20% was observed at day 6 with subsequent recovery, while following conventional irradiation, higher weight losses was observed with fewer instances of recovery. Concerning survival, all mice in the conventionally irradiated groups had a 100% mortality in the range of 15.5–18 Gy, while the mice irradiated with FLASH irradiation had a 100% survival in the same range. Conclusion: These results have demonstrated proof of principle that FLASH irradiations have a dramatic impact on the overall survival of mice following GI tract irradiations. If the increase in the therapeutic window can be validated and understood, this would revolutionize the field of radiation oncology and lead to increased cure rates with reduced side effects following treatment, resulting in increased quality of life for cancer survivors. Funding: DoD, Award#:W81XWH-14-1-0014, Weston Havens Foundation, Bio-X (Stanford University), the Office of the Dean of the Medical School, the Office of the Provost (Stanford University), and the Swedish Childhood Cancer Foundation; BL and PM are founders of TibaRay,Inc.; BL and PM have received research grants from Varian and RaySearch Laboratory.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2022

$$\alpha $$-event characterization and rejection in point-contact HPGe detectors

Abstract P-type point contact (PPC) HPGe detectors are a leading technology for rare event searches due to their excellent energy resolution, low thresholds, and multi-site event rejection capabilities. We have characterized a PPC detector’s response to $$\alpha $$ α particles incident on the sensitive passivated and p $$^+$$ + surfaces, a previously poorly-understood source of background. The detector studied is identical to those in the Majorana Demonstrator experiment, a search for neutrinoless double-beta decay ( $$0\nu \beta \beta $$ 0 ν β β ) in $$^{76}$$ 76 Ge. $$\alpha $$ α decays on most of the passivated surface exhibit significant energy loss due to charge trapping, with waveforms exhibiting a delayed charge recovery (DCR) signature caused by the slow collection of a fraction of the trapped charge. The DCR is found to be complementary to existing methods of $$\alpha $$ α identification, reliably identifying $$\alpha $$ α background events on the passivated surface of the detector. We demonstrate effective rejection of all surface $$\alpha $$ α events (to within statistical uncertainty) with a loss of only 0.2% of bulk events by combining the DCR discriminator with previously-used methods. The DCR discriminator has been used to reduce the background rate in the $$0\nu \beta \beta $$ 0 ν β β region of interest window by an order of magnitude in the Majorana Demonstrator and will be used in the upcoming LEGEND-200 experiment.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2016

Columbia County Habitat for Humanity Passive Townhomes

Columbia County (New York) Habitat for Humanity built a pair of townhomes to Passive House criteria with the purpose of exploring approaches for achieving Passive House performance and to eventually develop a prototype design for future projects. The project utilized a 2x6 frame wall with a structural insulated panel curtain wall and a ventilated attic over a sealed OSB ceiling air barrier. Mechanical systems include a single head, wall mounted ductless mini-split heat pump in each unit and a heat recovery ventilator. Costs were $26,000 per unit higher for Passive House construction compared with the same home built to ENERGY STAR version 3 specifications, representing about 18% of total construction cost. This report discusses the cost components, energy modeling results and lessons from construction. Two alternative ventilation systems are analyzed: a central system; and, a point-source system with small through-wall units distributed throughout the house. The report includes a design and cost analysis of these two approaches.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

NASA NTRS1990

Shape-memory properties in Ni-Ti sputter-deposited film

A Ni-Ti alloy, generically called nitinol, was prepared from sputtering targets of two different compositions on glass substrates using a dc magnetron source. The as-deposited films were amorphous in structure and did not exhibit a shape memory. The amorphous films were crystallized with a suitable annealing process, and the transformation properties were measured using differential scanning calorimetry. The annealed films demonstrated a strong shape-memory effect. Stress/strain measurements and physical manipulation were used to evaluate the shape recovery. These tests demonstrated sustained tensile stresses of up to 480 MPa in the high-temperature phase, and a characteristic plastic deformation in the low-temperature phase.

Busch, J. D.↗

NASA NTRS1993

Model-based reasoning for power system management using KATE and the SSM/PMAD

The overall goal of this research effort has been the development of a software system which automates tasks related to monitoring and controlling electrical power distribution in spacecraft electrical power systems. The resulting software system is called the Intelligent Power Controller (IPC). The specific tasks performed by the IPC include continuous monitoring of the flow of power from a source to a set of loads, fast detection of anomalous behavior indicating a fault to one of the components of the distribution systems, generation of diagnosis (explanation) of anomalous behavior, isolation of faulty object from remainder of system, and maintenance of flow of power to critical loads and systems (e.g. life-support) despite fault conditions being present (recovery). The IPC system has evolved out of KATE (Knowledge-based Autonomous Test Engineer), developed at NASA-KSC. KATE consists of a set of software tools for developing and applying structure and behavior models to monitoring, diagnostic, and control applications.

Morris, Robert A.↗

NASA NTRS1995

A novel photonic oscillator

We report a novel oscillator for photonic RF systems. This oscillator is capable of generating high-frequency signals up to 70 GHz in both electrical and optical domains and is a special voltage-controlled oscillator with an optical output port. It can be used to make a phase-locked loop (PLL) and perform all functions that a PLL is capable of for photonic systems. It can be synchronized to a reference source by means of optical injection locking, electrical injection locking, and PLL. It can also be self-phase locked and self-injection locked to generate a high-stability photonic RF reference. Its applications include high-frequency reference regeneration and distribution, high-gain frequency multiplication, comb-frequecy and square-wave generation, carrier recovery, and clock recovery. We anticipate that such photonic voltage-controlled oscillators (VCOs) will be as important to photonic RF systems as electrical VCOs are to electrical RF systems.

Yao, X. S.↗

NASA NTRS2002

Solid state 31phosphorus nuclear magnetic resonance of iron-, manganese-, and copper-containing synthetic hydroxyapatites

The incorporation of micronutrients into synthetic hydroxyapatite (SHA) is proposed for slow release of these nutrients to crops in the National Aeronautics and Space Administration's (NASA's) Advanced Life Support (ALS) program for Lunar or Martian outposts. Solid state 31P nuclear magnetic resonance (NMR) was utilized to examine the paramagnetic effects of Fe3+, Mn2+, and Cu2+ to determine if they were incorporated into the SHA structure. Separate Fe3+, Mn2+, and Cu2+ containing SHA materials along with a transition metal free SHA (pure-SHA) were synthesized using a precipitation method. The proximity (<1 nm) of the transition metals to the 31P nuclei of SHA were apparent when comparing the integrated 31P signal intensities of the pure-SHA (87 arbitrary units g-1) with the Fe-, Mn-, and Cu-SHA materials (37-71 arbitrary units g-1). The lower integrated 31P signal intensities of the Fe-, Mn-, and Cu-SHA materials relative to the pure-SHA suggested that Fe3+, Mn2+, and Cu2+ were incorporated in the SHA structure. Further support for Fe3+, Mn2+, and Cu2+ incorporation was demonstrated by the reduced spin-lattice relaxation constants of the Fe-, Mn-, and Cu-SHA materials (T'=0.075-0.434s) relative to pure-SHA (T1=58.4s). Inversion recovery spectra indicated that Fe3+, Mn2+, and Cu2+ were not homogeneously distributed about the 31P nuclei in the SHA structure. Extraction with diethylene-triamine-penta-acetic acid (DTPA) suggested that between 50 and 80% of the total starting metal concentrations were incorporated in the SHA structure. Iron-, Mn-, and Cu-containing SHA are potential slow release sources of Fe, Mn, and Cu in the ALS cropping system.

NASA Discipline Life Support Systems↗

NASA NTRS2002

Convergence of limb, visceral, and vertical semicircular canal or otolith inputs onto vestibular nucleus neurons

The major goal of this study was to determine the patterns of convergence of non-labyrinthine inputs from the limbs and viscera onto vestibular nucleus neurons receiving signals from vertical semicircular canals or otolith organs. A secondary aim was to ascertain whether the effects of non-labyrinthine inputs on the activity of vestibular nucleus neurons is affected by bilateral peripheral vestibular lesions. The majority (72%) of vestibular nucleus neurons in labyrinth-intact animals whose firing was modulated by vertical rotations responded to electrical stimulation of limb and/or visceral nerves. The activity of even more vestibular nucleus neurons (93%) was affected by limb or visceral nerve stimulation in chronically labyrinthectomized preparations. Some neurons received non-labyrinthine inputs from a variety of peripheral sources, including antagonist muscles acting at the same joint, whereas others received inputs from more limited sources. There was no apparent relationship between the spatial and dynamic properties of a neuron's responses to tilts in vertical planes and the non-labyrinthine inputs that it received. These data suggest that non-labyrinthine inputs elicited during movement will modulate the processing of information by the central vestibular system, and may contribute to the recovery of spontaneous activity of vestibular nucleus neurons following peripheral vestibular lesions. Furthermore, some vestibular nucleus neurons with non-labyrinthine inputs may be activated only during particular behaviors that elicit a specific combination of limb and visceral inputs.

NASA Discipline Developmental Biology↗

NASA NTRS2012

Application of Satellite Gravimetry for Water Resource Vulnerability Assessment

The force of Earth's gravity field varies in proportion to the amount of mass near the surface. Spatial and temporal variations in the gravity field can be measured via their effects on the orbits of satellites. The Gravity Recovery and Climate Experiment (GRACE) is the first satellite mission dedicated to monitoring temporal variations in the gravity field. The monthly gravity anomaly maps that have been delivered by GRACE since 2002 are being used to infer changes in terrestrial water storage (the sum of groundwater, soil moisture, surface waters, and snow and ice), which are the primary source of gravity variability on monthly to decadal timescales after atmospheric and oceanic circulation effects have been removed. Other remote sensing techniques are unable to detect water below the first few centimeters of the land surface. Conventional ground based techniques can be used to monitor terrestrial water storage, but groundwater, soil moisture, and snow observation networks are sparse in most of the world, and the countries that do collect such data rarely are willing to share them. Thus GRACE is unique in its ability to provide global data on variations in the availability of fresh water, which is both vital to life on land and vulnerable to climate variability and mismanagement. This chapter describes the unique and challenging aspects of GRACE terrestrial water storage data, examples of how the data have been used for research and applications related to fresh water vulnerability and change, and prospects for continued contributions of satellite gravimetry to water resources science and policy.

Rodell, Matthew↗