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DOE OSTI2015

CEA decommissioning and clean-up activities legacy waste management and lessons learned - 15506

The CEA has generated radioactive waste in both liquid and solid form for more than 50 years within the scope of its R and D, clean-up and dismantling programs. The vast majority of the waste produced is transferred to disposal centers in approved waste packages. Nonetheless, a large quantity of legacy waste still remains in ageing facilities in which the storage conditions are sometimes no longer satisfactory with respect to the safety requirements that are constantly evolving. As part of a broad clean-up and dismantling process focusing on these ageing facilities managed by the CEA, the top priority is to shut down nuclear activities on two symbolic sites: Grenoble and Fontenay-aux-Roses, which are both located in a dense urban environment. After about ten years of dismantling, the nuclear facilities on the Grenoble site are on their way to be completely decommissioned in the regulatory sense of the term. Furthermore, the radwaste issue on this site has raised no specific problems, though it did require developing innovative and sometimes costly waste outlets. The older Fontenay-aux-Roses site is where the first experimental research on minor actinide separation took place. The facilities on this site have reached a stage in dismantling which necessitates the recovery of irradiating legacy waste containing alpha, beta and gamma emitters. The transfer of this waste to interim storage centers more than 600 kilometers away is a decisive factor in reducing the site's nuclear source term and in ensuring the satisfactory progress of the dismantling operations. This paper details the issues raised by the recovery of legacy waste, which requires greater characterization to better understand its radiological and chemical status. This waste also requires better characterization to meet the storage requirements of new sites designed for storage periods exceeding 50 years prior to its final disposal in a deep geological repository. The issue of transporting waste on public roads is specifically covered, along with the strategy defined to securely transfer all legacy waste resulting from the CEA's very diverse R and D programs. Emphasis is placed on finding the right balance between collecting the necessary data on the waste to be transported, ensuring the reconditioning of this waste so it can be transported safely, and maintaining an efficient industrial-scale waste transfer process to limit the lead times and costs related to legacy waste recovery operations. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2024

Assessment of Accelerated Stress Testing Data for Silicon Photovoltaics Using Tensor Decomposition Methods

The photovoltaic (PV) industry is simultaneously targeting long warranties and new materials/designs for high-energy-yield modules, requiring an advanced methodology to forecast long-term durability of products with un-proven materials combinations. Extended, sequential, and combined stress testing methods are gaining popularity for assessing durability of PV modules/materials beyond the early-stage mortalities. Importantly, multiple degradation mechanisms can proceed simultaneously, and their separate contributions to the overall power loss should ideally be quantified. This work examines the use of data-driven tools towards developing a strategy for faster learning cycles in accelerated stress testing.

accelerated stress testing↗

DOE OSTI2015

Zeolite membrane cascade for tritium extraction and recovery systems

Membrane separation by zeolite membranes has been proposed as a pre-concentration stage for the tritium extraction from the purge helium of the breeding blanket combined with a final recovery by the catalytic membrane reactor PERMCAT. This fully continuous operation improves the tritium management in fusion machines, minimizing the tritium inventory. For the first time, the permeation measurements for H{sub 2} - He mixtures through a MFI-alumina hollow fibre membrane has been measured for different compositions (0.1 - 20% H{sub 2}) and temperatures. Such a highly permeable membrane, although it shows a limited selectivity, appears attractive for tritium recovery in the blanket. This will imply its operation in a membrane cascade, for which simulation work is ongoing. Mathematically the process is modeled using mass balance equations that can be transformed into the matrix form and solved iteratively assuming a permeate concentration on the first step of iteration, until the separation requirements are fulfilled.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

NASA NTRS1993

Investigation of aerodynamic design issues with regions of separated flow

Existing aerodynamic design methods have generally concentrated on the optimization of airfoil or wing shapes to produce a minimum drag while satisfying some basic constraints such as lift, pitching moment, or thickness. Since the minimization of drag almost always precludes the existence of separated flow, the evaluation and validation of these design methods for their robustness and accuracy when separated flow is present has not been aggressively pursued. However, two new applications for these design tools may be expected to include separated flow and the issues of aerodynamic design with this feature must be addressed. The first application of the aerodynamic design tools is the design of airfoils or wings to provide an optimal performance over a wide range of flight conditions (multipoint design). While the definition of 'optimal performance' in the multipoint setting is currently being hashed out, it is recognized that given a wide range of flight conditions, it will not be possible to ensure a minimum drag constraint at all conditions, and in fact some amount of separated flow (presumably small) may have to be allowed at the more demanding flight conditions. Thus a multipoint design method must be tolerant of the existence of separated flow and may include some controls upon its extent. The second application is in the design of wings with extended high speed buffet boundaries of their flight envelopes. Buffet occurs on a wing when regions of flow separation have grown to the extent that their time varying pressures induce possible destructive effects upon the wing structure or adversely effect either the aircraft controllability or passenger comfort. A conservative approach to the expansion of the buffet flight boundary is to simply expand the flight envelope of nonseparated flow under the assumption that buffet will also thus be alleviated. However, having the ability to design a wing with separated flow and thus to control the location, extent and severity of the separated flow regions may allow aircraft manufacturers to gain an advantage in the early design stages of an aircraft, when configuration changes are relatively inexpensive to make. The goal of the summer research at NASA Langley Research Center (LaRC) was twofold: first, to investigate a particular airfoil design problem observed under conditions of strong shock induced flow separation on the upper surface of an airfoil at transonic conditions; and second, to suggest and investigate design methodologies for the prediction (or detection) and control of flow separation. The context of both investigations was to use an existing two dimensional Navier-Stokes flow solver and the constrained direct/iterative surface curvature (CDISC) design algorithm developed at LaRC. As a lead in to the primary task, it was necessary to gain a familiarity with both the design method and the computational analysis and to perform the FORTRAN coding needed to couple them together.

Gally, Tom↗

NASA NTRS2013

Method of Separating Oxygen From Spacecraft Cabin Air to Enable Extravehicular Activities

Extravehicular activities (EVAs) require high-pressure, high-purity oxygen. Shuttle EVAs use oxygen that is stored and transported as a cryogenic fluid. EVAs on the International Space Station (ISS) presently use the Shuttle cryo O2, which is transported to the ISS using a transfer hose. The fluid is compressed to elevated pressures and stored as a high-pressure gas. With the retirement of the shuttle, NASA has been searching for ways to deliver oxygen to fill the highpressure oxygen tanks on the ISS. A method was developed using low-pressure oxygen generated onboard the ISS and released into ISS cabin air, filtering the oxygen from ISS cabin air using a pressure swing absorber to generate a low-pressure (high-purity) oxygen stream, compressing the oxygen with a mechanical compressor, and transferring the high-pressure, high-purity oxygen to ISS storage tanks. The pressure swing absorber (PSA) can be either a two-stage device, or a single-stage device, depending on the type of sorbent used. The key is to produce a stream with oxygen purity greater than 99.5 percent. The separator can be a PSA device, or a VPSA device (that uses both vacuum and pressure for the gas separation). The compressor is a multi-stage mechanical compressor. If the gas flow rates are on the order of 5 to 10 lb (.2.3 to 4.6 kg) per day, the compressor can be relatively small [3 ~16 ~16 in. (.8 ~41 ~41 cm)]. Any spacecraft system, or other remote location that has a supply of lowpressure oxygen, a method of separating oxygen from cabin air, and a method of compressing the enriched oxygen stream, has the possibility of having a regenerable supply of highpressure, high-purity oxygen that is compact, simple, and safe. If cabin air is modified so there is very little argon, the separator can be smaller, simpler, and use less power.

Graf, John C.↗

DOE OSTI2013

Hydrogen Recovery and Carbon Dioxide Separation in Steam Methane Reformers (SBIR Phase II Final Report)

Approximately six trillion standard cubic feet (scf) of hydrogen are produced each year by steam reforming light hydrocarbons. The water gas shift portion of the process yields a hydrogen product containing significant quantities of by-products such as carbon dioxide. The hydrogen must be purified for further use and carbon dioxide, a primary global warming agent, should be captured for other applications or sequestration. Pressure swing adsorption (PSA) is often used to produce high-purity hydrogen. However, the tail gas coming out of PSA contains about 15% of the hydrogen produced from reforming, and is currently used as fuel for reformers. The overall goal of this DOE-funded SBIR project was to develop a membrane process to recover hydrogen from PSA tail gas. This process also produces liquid carbon dioxide for sequestration. In the Phase I project, polyamide polyether based membranes were developed and evaluated with pure gases and model mixed hydrogen containing gases. Two bench scale modules were fabricated from these membranes, and evaluated with pure gases. These membranes and modules provided high carbon dioxide permeance and high carbon dioxide/hydrogen selectivity. In the Phase II project, a modified polyamide polyether based membrane, Polaris (TM), was successfully developed, and the membrane permeances were greatly improved. Bench scale modules prepared from this membrane were tested in the laboratory. Industrial scale 8-inch diameter modules were prepared and tested at BP's Pascagoula Gas Processing Plant. The modules were exposed to high-pressure natural gas for three months in a long-term integrity test. The promising results in the laboratory and field tests have generated great interest in using Polaris (TM) membranes for carbon dioxide/hydrogen separations. The membranes and processes developed in this project are in the early stage of commercialization. This work has already resulted in the sale of one commercial membrane unit for carbon dioxide removal and hydrogen purification.

02 PETROLEUM↗

NASA NTRS2019

CHANGO: A Software Tool for Boost Stage Guidance of the Space Launch System Exploration Mission 1

The Day of Launch Initiation Load Update (DOLILU) System is the means by which the Space Launch System (SLS) Vehicle trajectory is designed, verified, and uploaded on the Day of Launch (DOL) in order to ensure a safe flight. Launch vehicles are designed to fly down a narrow angle of attack and sideslip angle corridor in order to keep them within structural load limits. The angle of attack and sideslip angle response to the launch vehicle experiences can vary significantly based upon the winds experienced on the DOL. SLS Boost Stage flight employs an open-loop guidance scheme through Solid Rocket Booster (SRB) separation. In the SLS open-loop scheme, the vehicle will fly a prescribed set of attitudes as a function of the change in altitude since launch. This set of reference attitude values and corresponding altitude reference independent values are designed with ground software using winds measured on the DOL with the goal of minimizing angle of attack and sideslip angle, thereby minimizing related ascent integrated vehicle structural loads. The table of Boost Stage attitude commands as a function of altitude gained since launch is called the chi table. A software tool called CHANGO (Chi Angle Optimizer) designs the Boost Stage chi table which is uploaded to the vehicle’s flight computer and used during ascent by the flight software (FSW). The wind and atmospheric conditions are measured prior to launch and pre-processed to become input to the CHANGO software along with a set of parameters developed in advance of the DOL. CHANGO’s target set consists of the heading and altitude rate at SRB separation determined well before launch by the Program to Optimize Simulated Trajectories (POST). CHANGO consists of a simplified three degree-of-freedom (3-DOF) simulation representing the SLS launch configuration. In general, the launch azimuth is strongly correlated with the heading at SRB separation, and the initial pitchover rate is strongly correlated with the altitude rate at SRB separation. CHANGO uses an adaptation of Powell’s method to vary the initial pitchover rate and launch azimuth to solve a 2-dimentional minimization problem. CHANGO’s trajectory simulation is phase-based, with flight events separating the phases. Each flight phase has different attitude alignment logic. CHANGO’s 3-DOF simulation starts when the vehicle’s thrust-to-weight ratio equals one, and ends at a pre-calculated SRB separation time.

Ahmad, Naeem↗

DOE OSTI2017

Size_resolved_ice_nucleating_particle_INP_concentrations_from_the_INPOP_campaign

Ground-based immersion mode ice nucleation measurements were conducted on samples collected at the US DOE ARM AMF3 in Oliktok Point, AK from 1 Mar to 31 May 2017. Samples were collected using a Davis Rotating-drum Unit for Monitoring (DRUM; DRUMAir, LLC) cascading impactor in 4 stages (i.e., size bins). Instrument information on the model used, the DA400, can be found at the DRUMAir website (http://www.drumair.com/). Stages A, B, C, and D, had particle size cuts at 2.96, 1.21, 0.34, and 0.15 µm in particle diameter. Strips of sample substrate (PFA, perfluoroalkoxy; McMaster) were adhered to each disc in each stage and coated with petrolatum to enable particles to stick on impact. The discs move slowly over time, such that aerosol loading is streaked onto the PFA. Every 24 hours, a blank is created on the PFA to separate daily samples. The pump typically pulled 25 lpm at the inlet with all the discs in place in each stage. Daily samples were collected for each of the four stages, equaling 36,000 total L of air per sample. Discs rotated for approximately 24 days before the sampling per strip was complete and changed to a new disc. Discs were stored frozen after collection. Following collection and transport from AMF3 to PI Creamean's laboratory in Boulder, CO, strips were removed from the discs and cut up to separate daily samples. Each daily portion of the strip was stored in separate sterile bags and stored in a standard commercial freezer until analysis (approximately 4 – 5 months after collection). Drop freezing assays (DFAs) were conducted on one daily sample per week of the study for all four stages, with daily samples analyzed from 22 - 29 May 2017. Immediately after removal from the freezer, 2 mL of ultrapure water was added with a single-use sterile syringe directly to the bags, then mixed using a vortex mixer for 2 hours at 500 rpm to resuspend particles from the PFA into the ultrapure water. Following sample preparation, another single-use syringe was used to create 100 aliquots on a 3-inch diameter copper plate, then covered with a transparent plastic dome. The drops were approximately the same volume (2.5 µL each), though careful inspection. The plate was cooled at approximately 3 – 10 K min-1 from room temperature until all drops froze on the plate. Temperature was measured by an Omega thermocouple probes and meter. Drop freezing was visually detected, but recorded through monitoring software to provide the time frozen, channel of the meter used, temperature, and cooling rate for each drop. Not all 100 drops were always detected; the total number of rows in each data file equals the number of drops recorded, which typically was > 80 %. Each sample was tested three times (i.e., a new set of 100 drops was created for each test). Data provided are files containing these parameters. From the freezing temperatures recorded, the fraction frozen can be calculated as can the estimated INP concentration per L of air using the equation from Vali (1971): [INPs] = −(ln(f)/Valiquot)*(Vsuspension/Vair) where f is the proportion of droplets not frozen, Valiquot is the volume of each aliquot (i.e., 2.5e-6 L), Vsuspension is the volume of the suspension (i.e., 0.002 L), and Vair is the volume of air per sample (i.e., 36000 L). Vali, G.: Quantitative Evaluation of Experimental Results an the Heterogeneous Freezing Nucleation of Supercooled Liquids, Journal of the Atmospheric Sciences, 28, 402-409, 1971.

4-stage DRUM aerosol collector (DA400),Aerosol imp↗

DOE OSTI2020

Can the GPM IMERG Final Product Accurately Represent MCSs’ Precipitation Characteristics over the Central and Eastern United States?

Mesoscale convective systems (MCSs) play an important role in water and energy cycles as they produce heavy rainfall and modify the radiative profile in the tropics and midlatitudes. An accurate representation of MCSs’ rainfall is therefore crucial in understanding their impact on the climate system. The V06B Integrated Multisatellite Retrievals from Global Precipitation Measurement (IMERG) half-hourly precipitation final product is a useful tool to study the precipitation characteristics of MCSs because of its global coverage and fine spatiotemporal resolutions. However, errors and uncertainties in IMERG should be quantified before applying it to hydrology and climate applications. This study evaluates IMERG performance on capturing and detecting MCSs’ precipitation in the central and eastern United States during a 3-yr study period against the radar-based Stage IV product. The tracked MCSs are divided into four seasons and are analyzed separately for both datasets. IMERG shows a wet bias in total precipitation but a dry bias in hourly mean precipitation during all seasons due to the false classification of nonprecipitating pixels as precipitating. These false alarm events are possibly caused by evaporation under the cloud base or the misrepresentation of MCS cold anvil regions as precipitating clouds by the algorithm. IMERG agrees reasonably well with Stage IV in terms of the seasonal spatial distribution and diurnal cycle of MCSs precipitation. A relative humidity (RH)-based correction has been applied to the IMERG precipitation product, which helps reduce the number of false alarm pixels and improves the overall performance of IMERG with respect to Stage IV.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2011

Monitoring Spacecraft Telemetry Via Optical or RF Link

A patent disclosure document discusses a photonic method for connecting a spacecraft with a launch vehicle upper-stage telemetry system as a means for monitoring a spacecraft fs health and status during and right after separation and deployment. This method also provides an efficient opto-coupled capability for prelaunch built-in-test (BIT) on the ground to enable more efficient and timely integration, preflight checkout, and a means to obviate any local EMI (electromagnetic interference) during integration and test. Additional utility can be envisioned for BIT on other platforms, such as the International Space Station (ISS). The photonic telemetry system implements an optical free-space link with a divergent laser transmitter beam spoiled over a significant cone angle to accommodate changes in spacecraft position without having to angle track it during deployment. Since the spacecraft may lose attitude control and tumble during deployment, the transmitted laser beam interrogates any one of several low-profile meso-scale retro-reflective spatial light modulators (SLMs) deployed over the surface of the spacecraft. The return signal beam, modulated by the SLMs, contains health, status, and attitude information received back at the launch vehicle. Very compact low-power opto-coupler technology already exists for the received signal (requiring relatively low bandwidths, e.g., .200 kbps) to enable transfer to a forward pass RF relay from the launch vehicle to TDRSS (Tracking and Data Relay Satellite System) or another recipient. The link would be active during separation and post-separation to monitor spacecraft health, status, attitude, or other data inventories until attitude recovery and ground control can be re-established. An optical link would not interfere with the existing upper stage telemetry and beacon systems, thus meeting launch vehicle EMI environmental constraints.

Fielhauer, K. B.↗

DOE OSTI2015

Mass transfer apparatus and method for separation of gases

A process and apparatus for separating components of a source gas is provided in which more soluble components of the source gas are dissolved in an aqueous solvent at high pressure. The system can utilize hydrostatic pressure to increase solubility of the components of the source gas. The apparatus includes gas recycle throughout multiple mass transfer stages to improve mass transfer of the targeted components from the liquid to gas phase. Separated components can be recovered for use in a value added application or can be processed for long-term storage, for instance in an underwater reservoir.

03 NATURAL GAS↗

DOE OSTI2018

Mass transfer apparatus and method for separation of gases

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2015

A versatile apparatus for the fine-tuned synthesis of cluster-based materials

In this paper, a custom-designed experimental setup for the fine-tuned synthesis of various cluster–based materials is presented. Providing custom-designed deposition stages and special sample holders it offers a high degree of control over the sample characteristics such as the cluster size, cluster amounts, and sample homogeneity in combination with high sample purity. The system is capable of producing thin films of pure clusters and various cluster-matrix combinations with cluster sizes ranging from single atoms up to aggregates of several thousand atoms. Two custom-designed deposition stages are available, one utilizes the full cluster beam, yielding micrograms of pure clusters within a few hours and the second one uses mass-separated clusters (mass-resolution between 2% and 10%), yielding nanograms of pure clusters in the same timescale. Furthermore, at the second deposition stage, a variety of matrix materials can be co-deposited at a controlled sample temperature between 153 K and 673 K. In order to prove the capabilities of the apparatus, a series of experiments with Fe clusters embedded in Ag matrices with different volume fractions of clusters were carried out. Energy dispersive X-ray spectroscopy measurements revealed that the amount of deposited clusters as well as the sample homogeneity can be controlled with an outstanding accuracy of 10%. Additional measurements of the magnetic properties indicated the presence of separated clusters for volume fractions of clusters around 2 volume percent (vol. %), while above this concentration (10 vol. %) a partial aggregation of the clusters was observed. It was also shown that the resulting thin films are nearly oxygen free, which ascertains that oxygen sensitive materials can be safely handled in this newly developed apparatus.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2013

Numerical analysis of three complex three-dimensional shock wave / turbulent boundary layer interaction flows

A set of Reynolds-averaged Navier-Stokes (RANS) computations with turbulence closure provided by the Spalart-Allmaras (SA) model have been carried out for prediction of shock-induced three-dimensional (3D) turbulent separated flows. The experimental data for different aerodynamic test configurations have been used for assessing credibility of the numerical method employed. Particularly, shock wave / turbulent boundary layer interactions (SWTBLI) in the vicinity of an asymmetric sharp double-fin (DF) with different (7° and 11°) deflection angles mounted on a flat plate and two conically sharp cylindrical bodies at varying interbody distances and nose cone angles 60° and 40° mounted over a flat plate at freestream Mach number 4, as well as a transonic fan stage operating in the near-stall regime are considered. The gas dynamic structure and topology of 3D separated flows, surface flow patterns, and pressure distributions as well as body aerodynamic force prediction are analyzed. A transonic fan stage operating in the near-stall regime and a possibility of applying flow control is investigated. High Performance Computing was employed to make high resolution computations of these flows possible, and advanced 3D visualization techniques were employed in order to improve understanding of the separating flow phenomena.

42 ENGINEERING↗

DOE OSTI2025

Vibroacoustic Process Monitoring of 5-Stage Centrifugal Contactors

Vibroacoustic monitoring was investigated to aid in informing process operators with parameters regarding aqueous separation techniques. These techniques have a wide range of applications including nuclear fuel reprocessing. A small-scale solvent extraction system was set up with five magnetic drive contactors and two piston pumps to collect realistic operation. Vibration sensors were placed on three of the contactors and both pumps, and a microphone was placed near the system. Contactor rotational speed and pump flow rate were varied with known values to compare against measured vibroacoustic signatures. Spectral analysis allowed for the determination of contactor rotational speed and the ratio of organic to aqueous flow rate, an important parameter for ensuring optimal extraction. Vibration metrics such as kurtosis and crest factor provided additional details regarding individual rotational speeds and have potential in examination of faults for predictive maintenance. Overall, results indicate the capability of vibroacoustic monitoring to improve operator awareness and process outcomes.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2018

From coherent to vibronic light harvesting in photosynthesis

Photosynthetic organisms are a remarkable example of nanoscale engineering and have mastered the process of solar energy harvesting over billions of years of evolution. Therefore, researchers seek insights from the light collection mechanisms of photosynthetic machinery. The initial energy transfer stage of photosynthesis, which begins with light absorption and leads to charge separation, is remarkably robust in conditions of strong energetic disorder, extreme physiological temperatures, and low light flux — very different from conventional solar conversion materials [1, 2, 3]. However, determining the key principles which are responsible for efficient conversion is a challenging task due to the complexity of the photosynthetic systems. The field encountered a fascinating lead in 2007 when oscillatory features were discovered in two-dimensional electronic spectroscopic data — the optical analogue of 2D NMR — and were assigned to quantum coherence between donor and acceptor electronic states [4 •• ]. In this review, we describe the evolution in our understanding of quantum effects in photosynthetic energy transfer. A vibronic model is described to demonstrate the current opinion on how quantum effects can optimize energy transfer.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2025

Incorporation of Oxygen Carrier Recycle into Large-Scale Production of Cu-Based Oxygen Carriers

One of the greatest challenges in the chemical looping combustion (CLC) of solid fuels is developing an oxygen carrier material that is reactive and attrition resistant and can be prepared at a reasonable cost. Recent efforts in oxygen carrier development have followed two primary approaches: (1) using natural ores, such as ilmenite, or (2) developing highly attrition-resistant and reactive synthetic materials. Both approaches have shortcomings, namely, the low reactivity and incompatibility of ores with solid fuel CLC and the high cost and low durability of synthetic materials. Here, a different approach is taken where attrition is assumed inevitable and the recycling of spent oxygen carrier materials is incorporated into oxygen carrier manufacture. For solid fuel CLC, Cu-based oxygen carriers are attrited and are collected with fly ash. Copper oxides are more reactive with nitric acid than most ash materials, meaning that a copper-nitrate-rich leachate can be generated. This copper nitrate stream could then be reused in oxygen carrier synthesis by impregnation. For proof of concept, leaching experiments were conducted to verify that copper oxides are selectively leached from ash-containing spent oxygen carriers. Several cases for process design are proposed based on the composition of spent materials, as the degree of copper oxidation and type of solid fuel dictate leaching residence times and general processing intensity. The four stages proposed here include impurity removal, copper leaching and recovery, solid–liquid separation, and evaporation/concentrating. The resulting process should be able to recover up to 95% of copper while minimizing inclusion of undesirable ash-based impurities.

anions↗

DOE OSTI2016

Anthropogenic plutonium-244 in the environment: Insights into plutonium’s longest-lived isotope

Owing to the rich history of heavy element production in the unique high flux reactors that operated at the Savannah River Site, USA (SRS) decades ago, trace quantities of plutonium with highly unique isotopic characteristics still persist today in the SRS terrestrial environment. Development of an effective sampling, processing, and analysis strategy enables detailed monitoring of the SRS environment, revealing plutonium isotopic compositions, e.g., 244 Pu, that reflect the unique legacy of plutonium production at SRS. This work describes the first long-term investigation of anthropogenic 244 Pu occurrence in the environment. Environmental samples, consisting of collected foot borne debris, were taken at SRS over an eleven year period, from 2003 to 2014. Separation and purification of trace plutonium was carried out followed by three stage thermal ionization mass spectrometry (3STIMS) measurements for plutonium isotopic content and isotopic ratios. Furthermore, significant 244 Pu was measured in all of the years sampled with the highest amount observed in 2003. The 244 Pu content, in femtograms (fg = 10 –15 g) per gram, ranged from 0.31 fg/g to 44 fg/g in years 2006 and 2003 respectively. In all years, the 244 Pu/ 239 Pu atom ratios were significantly higher than global fallout, ranging from 0.003 to 0.698 in years 2014 and 2003 respectively.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗