Search NASA⌕ Search

SEARCH · Search NASA

Results for “RADIOACTIVE AEROSOLS”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

In the nuclear explosion monitoring context, what is an anomaly?

Abstract In the early years of nuclear explosion monitoring, experts used downwind detections with meaningful ratios of radioactive species to identify an explosion. Today’s reality is sparse networks of radionuclide monitoring stations looking for weak signals. Analysts need to discriminate between industrial background radioactivity and nuclear explosion signals, even using the detection of one isotope. Aerosol and xenon measurements potentially related to nuclear tests in 2006 and 2013 announced by the Democratic People’s Republic of Korea and from worldwide civilian background radioactivity are considered when defining radionuclide detection anomalies to objectively guide the use of limited analyst resources and reduce the possibility of not detecting nuclear explosions.

Miley, Harry S.↗
DOE OSTI2019

Spatiotemporal Distribution of {sup 241}Am in the Vicinity of the Waste Isolation Pilot Plant - 19543

Environmental monitoring around nuclear facilities is essential for characterizing the baseline conditions that are critical for identifying releases and quantifying their effects, should they occur, and for assessing post-closure performance. The spatiotemporal distribution and transport behavior of {sup 241}Am in the vicinity of a deep geologic repository for transuranic waste were assessed using data spanning the pre-operational phase to the present, including an accidental radionuclide release in 2014. The {sup 241}Am background values of 0.027±0.109 μBq/m{sup 3} (aerosols), and 0.061±0.065 Bq/kg (soil), as well as the {sup 241}Am/{sup 239+240}Pu ratios of 0.41±0.06 (aerosols) and 0.38±0.04 (soil), are similar to global fallout values. Pre-operations concentrations of {sup 241}Am show a strong seasonal dependence, attributed to resuspension of soils contaminated by global fallout, with no contribution from the upwind Project Gnome site ({sup 241}Am/{sup 239+240}Pu =0.24±0.08). During the 2014 accidental release, aerosol concentrations of {sup 241}Am briefly increased to 115.2 μBq/m{sup 3} at an onsite monitoring station, and 81.4 μBq/m{sup 3} at a station ∼1 km downwind of the exhaust shaft, changing the {sup 241}Am/{sup 239+240}Pu from ∼0.37 to ∼10. However, some four years later, conditions have returned to background. Almost 90% of the {sup 241}Am inventory is the 0-5 cm soil layer and there is no evidence of concentrations above regulatory standards, or that can be attributed to waste disposal operations. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

Current limitations and challenges in nanowaste detection, characterisation and monitoring

Highlights: • First review on detection of nanomaterials in complex waste samples. • Focus on nanoparticles in solid, liquid and gaseous waste samples. • Summary of current applicable methods for nanowaste detection and characterisation. • Limitations and challenges of characterisation of nanoparticles in waste. - Abstract: Engineered nanomaterials (ENMs) are already extensively used in diverse consumer products. Along the life cycle of a nano-enabled product, ENMs can be released and subsequently accumulate in the environment. Material flow models also indicate that a variety of ENMs may accumulate in waste streams. Therefore, a new type of waste, so-called nanowaste, is generated when end-of-life ENMs and nano-enabled products are disposed of. In terms of the precautionary principle, environmental monitoring of end-of-life ENMs is crucial to allow assessment of the potential impact of nanowaste on our ecosystem. Trace analysis and quantification of nanoparticulate species is very challenging because of the variety of ENM types that are used in products and low concentrations of nanowaste expected in complex environmental media. In the framework of this paper, challenges in nanowaste characterisation and appropriate analytical techniques which can be applied to nanowaste analysis are summarised. Recent case studies focussing on the characterisation of ENMs in waste streams are discussed. Most studies aim to investigate the fate of nanowaste during incineration, particularly considering aerosol measurements; whereas, detailed studies focusing on the potential release of nanowaste during waste recycling processes are currently not available. In terms of suitable analytical methods, separation techniques coupled to spectrometry-based methods are promising tools to detect nanowaste and determine particle size distribution in liquid waste samples. Standardised leaching protocols can be applied to generate soluble fractions stemming from solid wastes, while micro- and ultrafiltration can be used to enrich nanoparticulate species. Imaging techniques combined with X-ray-based methods are powerful tools for determining particle size, morphology and screening elemental composition. However, quantification of nanowaste is currently hampered due to the problem to differentiate engineered from naturally-occurring nanoparticles. A promising approach to face these challenges in nanowaste characterisation might be the application of nanotracers with unique optical properties, elemental or isotopic fingerprints. At present, there is also a need to develop and standardise analytical protocols regarding nanowaste sampling, separation and quantification. In general, more experimental studies are needed to examine the fate and transport of ENMs in waste streams and to deduce transfer coefficients, respectively to develop reliable material flow models.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2024

Source term estimation using noble gas and aerosol samples

Algorithms that estimate the location, time, and magnitude of a point-source atmospheric release using remotely sampled air concentrations typically use data for a single chemical or radioactive isotope. Here, a Bayesian algorithm is presented that uses data from multiple radioactive isotopes that are all released in the same short-duration event. Data from noble gas and aerosol samplers can be used simultaneously in the model. Application to a large synthetic data set using four isotopes shows the new algorithm generally gives more accurate location and time estimates than a comparable model using a single isotope.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Prediction for Pressure Differential Across HEPA Filter Media Based on Media Characteristics and Particle Size Distribution

A new method for predicting the pressure drop across High Efficiency Particulate Air (HEPA) filter media is proposed based upon mass deposited onto the filter and known physical characteristics of the filter media. Detailed are the methods used in conjunction with current filter loading models to predict the pressure drop, as well as tests conducted to validate the methods. The benefit of a prediction model for practical use lies in the manufacturing and service life of nuclear grade HEPA filters. HEPA filters for use in nuclear facilities have a prescribed expiration date and a maximum allowable operating pressure drop. Therefore, the ability to predict the pressure drop across a filter and relate it to an expected length of service time can enable a reduction in wasted filters. This will allow for more informed decisions to be made based upon the dictated life cycle of the filters. Also, understanding and predicting how the pressure drop of HEPA filter media behaves as a function of physical characteristics and loaded mass can assist in future design and manufacturing of filter media. Currently, most existing pressure drop models are either computationally based or analytical methods relying on data gathered during tests. Neither are practical for prediction; the computational methods are difficult to implement, and the current analytical methods are more useful as tools for analysis. The current analytical model developed by Bergman et al. is based upon the pressure drop from each media fiber and modeling the deposited particles as newly formed fibers. Using Bergman's model and the media properties, air properties, and known aerosol particle size distribution, a pressure drop curve as a function of loaded mass can be created. This curve implies initial loading in the depth of the filter media with a transition to pure surface loading on the filter face, and a sensitivity to an evolving particle size distribution as mass continues to load onto the filter. To implement the predictive model, knowledge of the mean filter fiber diameter and porosity of the filter media is required. Traditionally, the mean fiber diameter is calculated as an effective diameter from prior media testing, however, in this study a Scanning Electron Microscope (SEM) technique is used to acquire this variable. Validation of the predictive model is provided by flat sheet media tests under a controlled environment with a measured particle size distribution of the challenge aerosol and shows reasonable preliminary agreement.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

GOTHIC Aerosol Source Depletion Studies

Pacific Northwest National Laboratory has continued work to develop an aerosol-laden flow modeling capability with the Generation of Thermal Hydraulic Information in Containment (GOTHIC TM ) computer code to perform simulations for thermal hydraulic conditions and aerosol transport and deposition in spent fuel casks. This report describes our recent work to expand our model that was originally developed in 2019 to allow for thermal characterization, carrier gas flow determination, and tracking of particulate behavior throughout the entire canister volume. This was achieved through conversion of decay heat source in all fuel tubes within the model from heaters to thermal conductors in GOTHIC as well as remeshing the internal volume of the canister. These model improvements allowed for simulations of base case scenarios for comparison of similar efforts by our collaborators with alternative tools at Sandia and Oak Ridge. Several characteristics of the GOTHIC code were elucidated by this effort and were documented for consideration in how the code is used for this effort moving forward. For instance, treatment of particle size distributions, initial spatial distributions, mesh gradients, and minimum volume concentrations were identified as important issues for consideration. Ultimately, the current version of the code is capable of tracking temperatures, flow rates, and particle behavior throughout the canister internal volume. This report presents predicted depletion times and preferred deposition patterns within the canister. Additionally, this report documents code performance and insights for further model development and use for comparisons to other codes and for predicting system behavior in experiments being performed and planned by our collaborators.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

Nuclear Waste Tank Emission Contributions to Particle Size Distribution

Pollutants from anthropogenic activities including industrial processes are ubiquitous to the environment. To understand the impact from industrial aerosol on climate and human health, industrial aerosol needs to be better characterized. Here, in this study, particle number concentrations were used as a proxy for atmospheric pollutants, which include both particles and gases. Particle concentration and size distribution were measured using a scanning mobility particle sizer (SMPS) approximately 4.5 km from primary industrial areas at the Savannah River Site in Aiken, SC. Industrial areas include numerous nuclear waste storage and processing tanks. The SMPS data were divided into two groups depending on the wind direction measured onsite to categorize transport from the industrial area or from elsewhere. Industrial contributions were found to have a higher concentration of particles with sizes less than 200 nm, 859 ± 564 cm -3 , in comparison to non-industrial attributed particles, 733 ± 495 cm -3 on average from March-July 2021. For sizes larger than 200 nm, industrial and non-industrial particles have a similar concentration, 89 ± 59 cm -3 and 99 ± 61 cm -3 , with non-industrial concentrations being slightly larger. To confirm that industrial particles could travel to the sampling location, air dispersion modeling was completed for specific case studies during the sampling period. The atmospheric dispersion modeling results confirmed that particles released at the industrial areas reached the sampling location when the wind direction was favorable for transport from the industrial areas. The greater concentration of smaller-sized particles in industrial emissions has implications for typical particulate measurements (PM2.5), heath impacts, and climatological influences.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2014

Effects of digestion, chemical separation, and deposition on Po-210 quantitative analysis

Polonium-210 is a radioactive isotope often used to study sedimentation processes, food chains, aerosol behavior, and atmospheric circulations related to environmental sciences. Materials for the analysis of Po-210 range from tobacco leaves or cotton fibers, to soils and sediments. The purpose of this work was to determine polonium losses from a variety of sample types (soil, cotton fiber, and air filter) due to digestion technique, chemical separation, and deposition method for alpha energy analysis. Results demonstrated that yields from a perchloric acid wet-ash were similar to that from a microwave digestion. Both were greater than the dry-ash procedure. The polonium yield from the perchloric acid wet ash was 87 ± 5%, the microwave digestion had a yield of 100 ± 7%, and the dry ash had a yield of 38 ± 5%. The chemical separation of polonium by an anion exchange resin was used only on the soil samples due to the complex nature of this sample. The yield of Po-209 tracer after chemical separation and deposition for alpha analysis was 83 ± 7% for the soil samples. Spontaneous deposition yields for the cotton and air filters were 87 ± 4% and 92 ± 6%, respectively. Based on the overall process yields for each sample type the amount of Po-210 was quantified using alpha energy analysis. The soil contained 0.18 ± 0.08 Bq/g, the cotton swipe contained 0.7 mBq/g, and the air filter contained 0.04 ± 0.02 mBq/g. High and robust yields of polonium are possible using a suitable digestion, separation, and deposition method.

Seiner, Brienne N.↗
DOE OSTI2011

Gypsum treated fly ash as a liner for waste disposal facilities

Fly ash has potential application in the construction of base liners for waste containment facilities. While most of the fly ashes improve in the strength with curing, the ranges of permeabilities they attain may often not meet the basic requirement of a liner material. An attempt has been made in the present context to reduce the hydraulic conductivity by adding lime content up to 10% to two selected samples of class F fly ashes. The use of gypsum, which is known to accelerate the unconfined compressive strength by increasing the lime reactivity, has been investigated in further improving the hydraulic conductivity. Hydraulic conductivities of the compacted specimens have been determined in the laboratory using the falling head method. It has been observed that the addition of gypsum reduces the hydraulic conductivity of the lime treated fly ashes. The reduction in the hydraulic conductivity of the samples containing gypsum is significantly more for samples with high amounts of lime contents (as high as 1000 times) than those fly ashes with lower amounts of lime. However there is a relatively more increase in the strengths of the samples with the inclusion of gypsum to the fly ashes at lower lime contents. This is due to the fact that excess lime added to fly ash is not effectively converted into pozzolanic compounds. Even the presence of gypsum is observed not to activate these reactions with excess lime. On the other hand the higher amount of lime in the presence of sulphate is observed to produce more cementitious compounds which block the pores in the fly ash. The consequent reduction in the hydraulic conductivity of fly ash would be beneficial in reducing the leachability of trace elements present in the fly ash when used as a base liner.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2012

Experimental and numerical analysis of metal leaching from fly ash-amended highway bases

Highlights: Black-Right-Pointing-Pointer This study is the evaluation of leaching potential of fly ash-lime mixed soils. Black-Right-Pointing-Pointer This objective is met with experimental and numerical analysis. Black-Right-Pointing-Pointer Zn leaching decreases with increase in fly ash content while Ba, B, Cu increases. Black-Right-Pointing-Pointer Decrease in lime content promoted leaching of Ba, B and Cu while Zn increases. Black-Right-Pointing-Pointer Numerical analysis predicted lower field metal concentrations. - Abstract: A study was conducted to evaluate the leaching potential of unpaved road materials (URM) mixed with lime activated high carbon fly ashes and to evaluate groundwater impacts of barium, boron, copper, and zinc leaching. This objective was met by a combination of batch water leach tests, column leach tests, and computer modeling. The laboratory tests were conducted on soil alone, fly ash alone, and URM-fly ash-lime kiln dust mixtures. The results indicated that an increase in fly ash and lime content has significant effects on leaching behavior of heavy metals from URM-fly ash mixture. An increase in fly ash content and a decrease in lime content promoted leaching of Ba, B and Cu whereas Zn leaching was primarily affected by the fly ash content. Numerically predicted field metal concentrations were significantly lower than the peak metal concentrations obtained in laboratory column leach tests, and field concentrations decreased with time and distance due to dispersion in soil vadose zone.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2013

Evaluating performance of high efficiency mist eliminators

Processing liquid wastes frequently generates off gas streams with high humidity and liquid aerosols. Droplet laden air streams can be produced from tank mixing or sparging and processes such as reforming or evaporative volume reduction. Unfortunately these wet air streams represent a genuine threat to HEPA filters. High efficiency mist eliminators (HEME) are one option for removal of liquid aerosols with high dissolved or suspended solids content. HEMEs have been used extensively in industrial applications, however they have not seen widespread use in the nuclear industry. Filtering efficiency data along with loading curves are not readily available for these units and data that exist are not easily translated to operational parameters in liquid waste treatment plants. A specialized test stand has been developed to evaluate the performance of HEME elements under use conditions of a US DOE facility. HEME elements were tested at three volumetric flow rates using aerosols produced from an iron-rich waste surrogate. The challenge aerosol included submicron particles produced from Laskin nozzles and super micron particles produced from a hollow cone spray nozzle. Test conditions included ambient temperature and relative humidities greater than 95%. Data collected during testing HEME elements from three different manufacturers included volumetric flow rate, differential temperature across the filter housing, downstream relative humidity, and differential pressure (dP) across the filter element. Filter challenge was discontinued at three intermediate dPs and the filter to allow determining filter efficiency using dioctyl phthalate and then with dry surrogate aerosols. Filtering efficiencies of the clean HEME, the clean HEME loaded with water, and the HEME at maximum dP were also collected using the two test aerosols. Results of the testing included differential pressure vs. time loading curves for the nine elements tested along with the mass of moisture and solid material on each element at final dP. Plots of overall filtering efficiencies for DOP (spherical aerosol) and dry surrogate (aspherical aerosols) at specified dPs were computed for each filter. Filtering efficiencies were determined as a function of particle size. Curves were also generated showing the most penetrating particle size as a function of dP. A preliminary set of tests was conducted to evaluate spray location, duration, pressure, and wash volume for in-place cleaning the interior surface (reducing dP) of the HEME element. A variety of nozzle designs were evaluated and test results demonstrated the potential to overload the HEME (saturate filter medium) resulting in very high dPs and extensive drain times. At least one combination of spray nozzle design, spray location on the surface of the element, and spray time/pressure was successful in achieving extension of operational life. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Aging of Concrete for the Evaluation of Repair Materials to Protect the Walls of the HCAEX Tunnel at Savannah River - 20301

H-Canyon, located in the Savannah River site, is a unique facility for chemical reprocessing of plutonium, highly-enriched uranium, and other radioactive materials. The exhaust gases of the H-Canyon are sent through the H-Canyon Exhaust (HCAEX) tunnel for contamination removal. Robotic inspections of the tunnel revealed significant degradation of the reinforced concrete structure that was associated with acid attack, and could compromise the structural stability of the tunnel. Thus, the identification and evaluation of potential repair materials that could be applied on the degraded walls to mitigate and prevent further degradation is of significant interest to the Department of Energy and the Savannah River representatives. This research effort has been divided into two phases: 1) Development and evaluation of aged concrete under accelerated aging conditions (which is the focus of this paper) and 2) Evaluation of potential repair materials applied on aged and non-aged concrete under simulated aggressive conditions. In order to develop and evaluate concrete samples exposed to accelerated aging conditions in simulated aggressive environments, a literature review of the HCAEX tunnel was conducted that included 1) characterization and extent of the concrete damage, 2) environmental conditions inside the tunnel and 3) primary deterioration mechanisms. In addition, potential coatings and/or repair materials for degraded concrete surfaces exposed to aggressive environments (primarily acidic) were selected from the literature review and the most common testing and measurements for evaluating acid attack phenomena, erosion, etc. were reviewed. From the literature review findings, a preliminary bench-scale test plan for the concrete aging was developed, including accelerated aging tests with aggressive conditions (acid fumes, humidity, etc.). Concrete samples were exposed to the aging accelerated conditions (e.g. immersion in acid solutions) and visual inspection, mass loss and pH change (acid solution) were recorded over time. Correlations between the visual inspection, mass loss and pH changes results and the aging time or the aging conditions were developed. Specimens submitted to the highest acid concentration showed the fastest and most intense degradation. The type of coarse aggregate (limestone) used for the concrete seemed to be the cause of the fastest aging observed, compared to the cement paste. The research findings created the foundation for the ongoing investigation, in which new concrete samples with a mix design similar to the HCAEX tunnel will be tested and will serve as the substrate for testing the selected coatings and /or repair materials. In this paper, the literature review and preliminary results from the aging tests are provided. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

Review of molten salt reactor off-gas management considerations

Molten salt reactors offer a wide range of potential benefits but pose some unique challenges, particularly for designs that use an unclad liquid salt fuel. This type of fuel will result in the transport of fission gases into the headspace of the reactor where in some designs a cover gas can be circulated to remove certain fission products and maintain an inert atmosphere. The cover gas leaving the reactor core is expected to contain both noble and non-noble gases, aerosols, volatile species, tritium, radionuclides, and their daughters. To remove these radioactive gases, it is necessary to develop a robust off-gas system for molten salt–fueled reactors. Various treatment systems must be staged in series to remove the off-gas constituents from the stream before recirculating the gas back to the headspace of the reactor. Treatment options vary greatly depending on what they are designed to remove from the gas stream. This paper reviews the anticipated composition of a typical molten salt reactor off-gas stream and subsequently the available resources that could be employed to remove these species from the gas stream. An example off-gas system is then detailed, along with important design considerations, exemplifying the necessity for high-fidelity modeling. Lastly, the need for further thermophysical property research and the employment of advanced sensor technology for treatment component testing are discussed.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2015

Evaluation of DUSTRAN Software System for Modeling Chloride Deposition on Steel Canisters

The degradation of steel by stress corrosion cracking (SCC) when exposed to atmospheric conditions for decades is a significant challenge in the fossil fuel and nuclear industries. SCC can occur when corrosive contaminants such as chlorides are deposited on a susceptible material in a tensile stress state. The Nuclear Regulatory Commission has identified chloride-induced SCC as a potential cause for concern in stainless steel used nuclear fuel (UNF) canisters in dry storage. The modeling of contaminant deposition is the first step in predictive multiscale modeling of SCC that is essential to develop mitigation strategies, prioritize inspection, and ensure the integrity and performance of canisters, pipelines, and structural materials. A multiscale simulation approach can be developed to determine the likelihood that a canister would undergo SCC in a certain period of time. This study investigates the potential of DUSTRAN, a dust dispersion modeling system developed by Pacific Northwest National Laboratory, to model the deposition of chloride contaminants from sea salt aerosols on a steel canister. Results from DUSTRAN simulations run with historical meteorological data were compared against measured chloride data at a coastal site in Maine. DUSTRAN’s CALPUFF model tended to simulate concentrations higher than those measured; however, the closest estimations were within the same order of magnitude as the measured values. The decrease in discrepancies between measured and simulated values as the level of abstraction in wind speed decreased suggest that the model is very sensitive to wind speed. However, the influence of other parameters such as the distinction between open-ocean and surf-zone sources needs to be explored further. Deposition values predicted by the DUSTRAN system were not in agreement with concentration values and suggest that the deposition calculations may not fully represent physical processes. Overall, results indicate that with parameter refinement, DUSTRAN has the potential to simulate atmospheric chloride dispersion on steel canisters.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Monitoring Xenon Capture in a Metal Organic Framework Using Laser-Induced Breakdown Spectroscopy

Molten salt reactor operation will necessitate circulation of a cover gas to remove certain evolved fission products and maintain an inert atmosphere. The cover gas leaving the reactor core is expected to contain both noble and non-noble gases, aerosols, volatile species, tritium, and radionuclides and their daughters. To remove these radioactive gases, it is necessary to develop a robust off-gas system, along with novel sensors to monitor the gas stream and the treatment system performance. In this study, a metal organic framework (MOF) was engineered for the capture of Xe, a major contributor to the off-gas source term. The engineered MOF column was tested with a laser-induced breakdown spectroscopy (LIBS) sensor for noble gas monitoring. The LIBS sensor was used to monitor breakthrough tests with various Xe, Kr, and Ar mixtures to determine the Xe selectivity of the MOF column. This study offers an initial demonstration of the feasibility of monitoring off-gas treatment systems using a LIBS sensor to aid in the development of new capture systems for molten salt reactors.

47 OTHER INSTRUMENTATION↗
DOE OSTI2019

Development of a Trace Detection Method for Mercury Speciation in Hanford Tank Waste - 19014

The U.S. Department of Energy's (DOE) Hanford Site in southeast Washington State stores 56 million gallons of chemical and radioactive waste stored in underground tanks. Mercury species in liquid and solid fractions of Hanford tank waste pose a risk to the implementation and execution of DoE's River Protection Project mission due to mercury concentration limits imposed under waste acceptance criteria, toxicity characteristic leaching procedure restrictions for secondary waste disposal, and air emission permits. Although there is currently no processing of tank waste at Hanford, waste processing is imminent, and representative mercury inventory tracking will be important to anticipate and mitigate stack emissions and secondary liquid waste disposal issues. A methodology to accurately determine total mercury and mercury speciation in Hanford tank waste, while maintaining low mercury detection limits, currently does not exist at Hanford. Moreover, the mercury species in the waste solids are unknown and may be waste type-specific. The development of an analytical method to separate and speciate mercury in tank waste was undertaken by the Pacific Northwest National Laboratory (PNNL) while leveraging an existing non-radiological, ultra-trace mercury detection technique frequently performed at PNNL's Marine Sciences Laboratory in Sequim, Washington. The ultimate goal of this work is to develop an analytical method to obtain detailed mercury speciation information and update flowsheet modeling assumptions related to mercury partitioning at Hanford. The first phase of testing was completed in the development of an analytical methodology for the low-level determination of total mercury, elemental mercury, methylmercury, and dimethylmercury in Hanford tank waste. This paper presents Phase I testing which focused on determining whether mercury species can be preconcentrated from aqueous Hanford tank waste solution onto a solid substrate, while simultaneously eliminating or very significantly reducing the parent radionuclide activity. This was demonstrated by developing protocols for the separation and preconcentration of total mercury and methylmercury onto solid substrates, then measuring the substrates for radiological content at PNNL's Radiochemical Processing Laboratory on the Hanford Site. The mercury content was successfully separated onto stable substrates and the radionuclide activity reduction was significant enough that the preconcentrated samples could be subjected to quantification using far less restrictive handling and radiological controls than would be required for the parent sample (i.e., contamination area fume hood vs. hot cell). This mercury separation method required no sample dilution, which enables maximum mercury detectability, while still allowing mercury speciation. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗