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In Situ Mercury Stabilization (ISMS) Treatment: Technology Maturation Project Phase I Status Report

Description: Mercury (Hg) was used to separate lithium-6 isotope for weapons production at the Y-12 Plant in Oak Ridge in the 1950s and 1960s. As much as two million pounds of elemental mercury was 'lost' or unaccounted for and a large portion of that material is believed to have entered the environment. The DOE site office in Oak Ridge has identified Hg pollution in soils, sediments, and streams as the most significant environmental challenge currently faced. In industry, large amounts of mercury have been used to manufacture products (e.g., fluorescent light bulbs, thermometers) and for chemical processing (e.g., production of chlorine and alkali via mercury electrochemical cells) and many of these industrial sites are now polluted with mercury contaminated soil as a result of previous releases and/or inadvertent leaks. Remediation techniques for Hg contaminated soils are either based on thermal desorption and recovery of the mercury or excavation and shipping of large volumes of material to remote facilities for treatment and disposal. Both of these alternatives are extremely costly. The Brookhaven National Laboratory (BNL) Environmental Research & Technology Division (ERTD) has demonstrated, in laboratory-scale experiments, the viability of treating mercury contaminated soils by means of sulfide treatment rods inserted into the soil through a process known as In Situ Mercury Stabilization (ISMS). This approach is partly based on BNL's patented and successfully licensed ex situ process for Hg treatment, Sulfur Polymer Stabilization/Solidification (SPSS) which converts Hg to the more stable sulfide form. The original experiments showed that Hg homogeneously distributed in soil rapidly migrates to form a high concentration zone of chemically stable mercuric sulfide near the treatment rods while concentrations of Hg in surrounding areas away from the treatment rods are depleted to acceptable levels. BSA has subsequently filed for patent protection on the ISMS technology. If further developed it ...
Date: March 1, 2008
Creator: Kalb,P.D. & Milian, L.
Partner: UNT Libraries Government Documents Department

Laboratory evaluation of performance and durability of polymer grouts for subsurface hydraulic/diffusion barriers. Informal report, October 1993--May 1994

Description: Contaminated soils, buried waste and leaking underground storage tanks pose a threat to the environment through contaminant transport. One of the options for control of contaminant migration from buried waste sites is the construction of a subsurface barrier. Subsurface barriers increase the performance of waste disposal sites by providing a low permeability layer that can reduce percolation water migration into the waste site, minimize surface transport of contaminants, and reduce migration of volatile species. Also, a barrier can be constructed to envelop the site or plume completely, there by containing the contaminants and the potential leakage. Portland cement grout curtains have been used for barriers around waste sites. However, large castings of hydraulic cements result invariably in cracking due to shrinkage, thermal stresses induced by the hydration reactions, and wet-dry cycling prevalent at and sites. Therefore, improved, low permeability, high integrity materials are under investigation by the Department of Energy`s (DOE) Office of Technology Development, Integrated Demonstrations and Programs. The binders chosen for characterization include: an acrylic, a vinylester styrene, bitumen, a polyester styrene, furfuryl alcohol, and sulfur polymer cement. These materials cover broad ranges of chemical and physical durability, performance, viscosity, and cost. This report details the results of laboratory formulation, testing, and characterization of several innovative polymer grouts. An appendix containing a database of the barrier materials is at the end of this report.
Date: May 1, 1994
Creator: Heiser, J.H. & Milian, L.W.
Partner: UNT Libraries Government Documents Department

Leaching studies of low-level radioactive waste forms

Description: A research program has been under way at the Brookhaven National Laboratory to investigate the radionuclide release behavior of ion exchange bead resin waste solidified in Portland cement. An important aspect of this program is to develop and evaluate testing procedures and methodologies which enable the long-term performance evaluation of waste forms under simulated field conditions. Cesium and strontium release behavior using a range of testing procedures, including intermittent leachant flow conditions, has been investigated. For cyclic wet/dry leaching tests, extended dry periods tend to enhance the release of Cs and suppress the release of Sr. Under extended wet period leaching conditions, however, both Cs and Sr exhibit suppressed releases. In contrast, radionuclide releases observed under continuously saturated leaching conditions, as represented by conventional leaching tests, are significantly different. The relevance and aplicability of these laboratory data obtained under a wide range of leaching conditions to the performance evaluation of waste forms under anticipated field conditions is discussed. 12 refs., 9 figs., 3 tabs.
Date: January 1, 1985
Creator: Dayal, R.; Arora, H.; Clinton, J.C. & Milian, L.
Partner: UNT Libraries Government Documents Department

Leaching studies of low-level radioactive waste forms

Description: A research program has been underway at the Brookhaven National Laboratory to investigate the release of radionuclides from low-level waste forms under laboratory conditions. This paper describes the leaching behavior of Cs-137 from two major low-level waste streams, that is, ion exchange bead resin and boric acid concentrate, solidified in Portland cement. The resultant leach data are employed to evaluate and predict the release behavior of Cs-137 from low-level waste forms under field burial conditions.
Date: January 1, 1985
Creator: Dayal, R.; Arora, H.; Milian, L. & Clinton, J.
Partner: UNT Libraries Government Documents Department

Correlation of /sup 137/Cs leachability from small-scale to large-scale waste forms

Description: A study correlating the leachability of /sup 137/Cs from small-scale to large-scale cement forms was performed. The waste forms consisted of (a) organic ion exchange resins incorporated in Portland I cement, with a waste-to-cement ratio of 0.6 and a water-to-cement ratio of 0.4 (as free water) and (b) boric acid waste (12% solution) incorporated in Portland III cement, with a waste-to-cement ratio of 0.7. /sup 137/Cs was added to both waste types prior to solidification. The sample dimensions varied from 1 in. x 1 in. to 22 in. x 22 in. (diameter x height). Leach data extending over a period of 260 days were obtained using a modified IAEA leach test. A method based on semi-infinite plane source diffusion model was applied to interpret the leach data. A derived mathematical expression allows prediction of the amount of /sup 137/Cs leached from the forms as a function of leaching time and waste form dimensions. A reasonably good agreement between the experimental and calculated data was obtained. 4 figures, 6 tables.
Date: January 1, 1982
Creator: Morcos, N.; Dayal, R.; Milian, L. & Weiss, A.J.
Partner: UNT Libraries Government Documents Department

Sulfur Polymer Stabilization/Solidification Treatability Study of Mercury Contaminated Soil from the Y-12 Site

Description: As a result of past operations, the Department of Energy’s (DOE) Oak Ridge Y-12 National Security Complex (Y-12 Plant) has extensive mercury-contamination in building structures, soils, storm sewer sediments, and stream sediments, which are a source of pollution to the local ecosystem. Because of mercury’s toxicity and potential impacts on human health and the environment, DOE continues to investigate and implement projects to support the remediation of the Y-12 site.URS and #9122;CH2M Oak Ridge LLC (UCOR) under its prime contract with DOE has cleanup responsibilities on the DOE Oak Ridge Reservation and is investigating potential mercury-contaminated soil treatment technologies through an agreement with Babcock and Wilcox (B and W) Y-12, the Y-12 operating contractor to DOE. As part of its investigations, UCOR has subcontracted with Brookhaven National Laboratory (BNL) to conduct laboratory-scale studies evaluating the applicability of the Sulfur Polymer Stabilization/Solidification (SPSS) process using surrogate and actual mixed waste Y-12 soils containing mercury (Hg) at 135, 2,000, and 10,000 ppm.SPSS uses a thermoplastic sulfur binder to convert Hg to stable mercury sulfide (HgS) and solidifies the chemically stable product in a monolithic solid final waste form to reduce dispersion and permeability. Formulations containing 40 – 60 dry wt% Y-12 soil were fabricated and samples were prepared in triplicate for Environmental Protection Agency Toxicity Characteristic Leaching Procedure (TCLP) testing by an independent laboratory. Those containing 50 and 60 wt% soil easily met the study criteria for maximum allowable Hg concentrations (47 and 1 ppb, respectively compared with the TCLP limit of 200 ppb Hg). The lowest waste loading of 40 wt% yielded TCLP Hg concentrations slightly higher (240 ppb) than the allowable limit. Since the Y-12 soil tended to form clumps, the improved leaching at higher waste loadings was probably due to reduction in particle size from friction of the soil ...
Date: November 30, 2012
Creator: Kalb, P.; Milian, L. & Yim, S. P.
Partner: UNT Libraries Government Documents Department


Description: The BGRR was the world's first nuclear reactor dedicated to the peaceful exploration of atomic energy. The reactor pile consisted of a 700-ton, 25-foot cube of graphite fueled by uranium. A total of 1,369 fuel channels were available with roughly half in use at any given time. Insertion and removal of boron steel control rods controlled reactor power levels. One or more of five fans powered air-cooling. Air was brought in through two filtered plenums, flowed through and around the reactor core, through an exhaust duct containing filters, and finally out through the 320-foot high exhaust stack. Spent fuel was temporarily stored in the spent-fuel canal, and then sent to the Department of Energy's Savannah River Site (SRS). Access to the canal for removing spent fuel was through the Canal House (Building 709). The BGRR ceased operation in 1968 and was placed in a shutdown mode in which all fuel was removed and sent to SRS. Penetrations in the biological shield around the graphite cube and fuel channels were sealed. The final decontamination and decommissioning (D and D) process was initiated in 1999 and is scheduled for completion in 2005. An accelerated schedule was developed that combines characterization with removal actions for the various systems and structures. Before D and D work on a section of the BGRR facility begins, contaminant characterization is conducted to determine the types and amounts of contaminants present. The data are then used for project planning, including decisions affecting the extent of removal, waste designation, and health and safety plans.
Date: December 1, 2001
Partner: UNT Libraries Government Documents Department

Sulfur polymer stabilization/solidification (SPSS) treatment of mixed waste mercury recovered from environmental restoration activities at BNL

Description: Over 1,140 yd{sup 3} of radioactively contaminated soil containing toxic mercury (Hg) and several liters of mixed-waste elemental mercury were generated during a Comprehensive Environmental Response, Compensation and Liability Act (CERCLA) removal action at Brookhaven National Laboratory (BNL). The US Department of Energy's (DOE) Office of Science and Technology Mixed Waste Focus Area (DOE MWFA) is sponsoring a comparison of several technologies that may be used to treat these wastes and similar wastes at BNL and other sites across the DOE complex. This report describes work conducted at BNL on the application and pilot-scale demonstration of the newly developed Sulfur Polymer Stabilization/Solidification (SPSS) process for treatment of contaminated mixed-waste soils containing high concentrations ({approximately} 5,000 mg/L) of mercury and liquid elemental mercury. BNL's SPSS (patent pending) process chemically stabilizes the mercury to reduce vapor pressure and leachability and physically encapsulates the waste in a solid matrix to eliminate dispersion and provide long-term durability. Two 55-gallon drums of mixed-waste soil containing high concentrations of mercury and about 62 kg of radioactive contaminated elemental mercury were successfully treated. Waste loadings of 60 wt% soil were achieved without resulting in any increase in waste volume, while elemental mercury was solidified at a waste loading of 33 wt% mercury. Toxicity Characteristic Leaching Procedure (TCLP) analyses indicate the final waste form products pass current Environmental Protection Agency (EPA) allowable TCLP concentrations as well as the more stringent proposed Universal Treatment Standards. Mass balance measurements show that 99.7% of the mercury treated was successfully retained within the waste form, while only 0.3% was captured in the off gas system.
Date: January 29, 2001
Creator: Kalb, P.; Adams, J. & Milian, L.
Partner: UNT Libraries Government Documents Department


Description: The Brookhaven Graphite Research Reactor is currently on an accelerated decommissioning schedule with a completion date projected for 2005. The accelerated schedule combines characterization with removal actions for the various systems and structures. A major project issue involves characterization of the soils beneath contaminated Below Grade Ducts (BGD), the main air ducts connecting the exhaust plenums with the Fan House. The air plenums experienced water intrusion during BGRR operations and after shutdown. The water intrusions were attributed to rainwater leaks into degraded parts of the system, and to internal cooling water system leaks. If the characterization could provide enough information to show that soil contamination surrounding the BGD is either below cleanup guidelines or is very localized and can be ''surgically removed'' at a reasonable cost, the ducts may be decontaminated and left in place. This will provide significant savings compared to breaking up the 170-ft. long concrete duct, shipping the projected 9,000 m{sup 3} of waste off-site and disposing of it in an approved site. The focus of this Department of Energy Accelerated Site Technology Deployment (DOE ASTD) project was to determine the extent (location, type, and level) of soil contamination surrounding the BGD. A suite of innovative characterization tools was used to complete the characterization of the soil surrounding the BGD in a cost-effective and timely fashion and in a manner acceptable to the stakeholders. A state-of-the-art perfluorocarbon tracer (PFT) technology was used to screen the BGD for existing leak pathways and thus focus the characterization on potential contamination ''hot spots.'' Once pathways were identified, the sampling and analysis plan was designed to emphasize the leaking areas of the duct and perform only confirmatory checks in areas shown to be leak-free. A small-footprint Geoprobe{reg_sign} was used obtain core samples and allowed sampling in areas surrounding the BGD that ...
Date: August 4, 2002
Partner: UNT Libraries Government Documents Department

Properties and solidification of decontamination wastes

Description: LWRs will require one or more chemical decontaminations to achieve their designed lifetimes. Primary system decontamination is designed to lower radiation fields in areas where plant maintenance personnel must work. Chemical decontamination methods are either hard (concentrated chemicals, approximately 5 to 25 weight percent) or soft (dilute chemicals less than 1 percent by weight). These methods may have different chemical reagents, some tailor-made to the crud composition and many methods are and will be proprietary. One factor common to most commercially available processes is the presence of organic acids and chelates. These types of organic reagents are known to enhance the migration of radionuclides after disposal in a shallow land burial site. The NRC sponsors two programs at Brookhaven National Laboratory that are concerned with the management of decontamination wastes which will be generated by the full system decontamination of LWRs. These two programs focus on potential methods for degrading or converting decontamination wastes to more acceptable forms prior to disposal and the impact of disposing of solidified decontamination wastes. The results of the solidification of simulated decontamination resin wastes will be presented. Recent results on combustion of simulated decontamintion wastes will be described and procedures for evaluating the release of decontamination reagents from solidified wastes will be summarized.
Date: January 1, 1983
Creator: Davis, M.S.; Piciulo, P.L.; Bowerman, B.S.; Adams, J.W. & Milian, L.
Partner: UNT Libraries Government Documents Department

Demonstration of the BNL Continuous Dual Trap Analyzer to Detect Perfluorocarbon Tracers for the Tag, Track and Location Program

Description: The Tag, Track and Location System (TTL) Program is investigating methods of tracking an asset using perfluorocarbon tracers (PFT). The success of any TTL method requires sound detection/location instrumentation. Tracer Detection Technologies Corp (TDT), through a contract with the Office of Naval Research (ONR), is investigating different detection systems. The detections systems generally fall into two categories; proximity detectors and standoff detectors. Proximity detectors, as the name implies, need to be in close proximity (e.g., meter to 10's of meters) to the PFT source. Standoff detection searches for the PFT from a greater distance away from the source (e.g., 100's of meters to kilometers). Gas Chromatographs (GC) are generally considered a proximity detection systems, but in the case of PFTs should be considered for both proximity and standoff detection with the caveat that in standoff use the GC needs to be somewhere in the PFT plume, i.e., generally downwind of the source. With a properly sized PFT source, the right GC can afford fairly large standoff (distance from the source) distances; 100's of meters to kilometers downwind. Brookhaven National Laboratory (BNL) has such a GC system and offered to demonstrate the CDTA for TTL as a no cost addition to the TDTTTL project, of which BNL was a participant. BNL is a leading authority on the sampling, collection, release and detection of PFTs. In addition, the BNL team has extensive background in atmospheric dispersion, the application of PFTs to such studies and the development of applications utilizing PFTs such as building infiltration measurements, control room integrity determination, leak location and environmental investigations. This experience and expertise is essential in developing any PFT application were dispersion, dilution and overcoming environmental conditions and interferences are integral to success. BNL has developed sophisticated gas chromatography methods and instruments that allow detection of up ...
Date: October 7, 2008
Creator: Heiser,J.H.; Adams, J.; Dietz, R..; Milian, L. & Watson, T.
Partner: UNT Libraries Government Documents Department

Subsurface barrier integrity verification using perfluorocarbon tracers

Description: Subsurface barriers are an extremely promising remediation option to many waste management problems. Gas phase tracers include perfluorocarbon tracers (PFT`s) and chlorofluorocarbon tracers (CFC`s). Both have been applied for leak detection in subsurface systems. The focus of this report is to describe the barrier verification tests conducted using PFT`s and analysis of the data from the tests. PFT verification tests have been performed on a simulated waste pit at the Hanford Geotechnical facility and on an actual waste pit at Brookhaven National Laboratory (BNL). The objective of these tests were to demonstrate the proof-of-concept that PFT technology can be used to determine if small breaches form in the barrier and for estimating the effectiveness of the barrier in preventing migration of the gas tracer to the monitoring wells. The subsurface barrier systems created at Hanford and BNL are described. The experimental results and the analysis of the data follow. Based on the findings of this study, conclusions are offered and suggestions for future work are presented.
Date: December 1, 1996
Creator: Sullivan, T.M.; Heiser, J.; Milian, L. & Senum, G.
Partner: UNT Libraries Government Documents Department

BNL Building 650 lead decontamination and treatment feasibility study. Final report

Description: Lead has been used extensively at Brookhaven National Laboratory (BNL) for radiation shielding in numerous reactor, accelerator and other research programs. A large inventory of excess lead (estimated at 410,000 kg) in many shapes and sizes is currently being stored. Due to it`s toxicity, lead and soluble lead compounds are considered hazardous waste by the Environmental Protection Agency. Through use at BNL, some of the lead has become radioactive, either by contamination of the surface or through activation by neutrons or deuterons. This study was conducted at BNL`s Environmental and Waste Technology Center for the BNL Safety and Environmental Protection Division to evaluate feasibility of various treatment options for excess lead currently being stored. The objectives of this effort included investigating potential treatment methods by conducting a review of the literature, developing a means of screening lead waste to determine the radioactive characteristics, examining the feasibility of chemical and physical decontamination technologies, and demonstrating BNL polyethylene macro-encapsulation as a means of treating hazardous or mixed waste lead for disposal. A review and evaluation of the literature indicated that a number of physical and chemical methods are available for decontamination of lead. Many of these techniques have been applied for this purpose with varying degrees of success. Methods that apply mechanical techniques are more appropriate for lead bricks and sheet which contain large smooth surfaces amenable to physical abrasion. Lead wool, turnings, and small irregularly shaped pieces would be treated more effectively by chemical decontamination techniques. Either dry abrasion or wet chemical methods result in production of a secondary mixed waste stream that requires treatment prior to disposal.
Date: October 1, 1995
Creator: Kalb, P.D.; Cowgill, M.G. & Milian, L.W.
Partner: UNT Libraries Government Documents Department

Treatability study on the use of by-product sulfur in Kazakhstan for the stabilization of hazardous and radioactive wastes

Description: The Republic of Kazakhstan generates significant quantities of excess sulfur from the production and refining of petroleum reserves. In addition, the country also produces hazardous, and radioactive wastes which require treatment/stabilization. In an effort to find secondary uses for the elemental sulfur, and simultaneously produce a material which could be used to encapsulate, and reduce the dispersion of harmful contaminants into the environment, BNL evaluated the use of the sulfur polymer cement (SPC) produced from by-product sulfur in Kazakhstan. This thermoplastic binder material forms a durable waste form with low leaching properties and is compatible with a wide range of waste types. Several hundred kilograms of Kazakhstan sulfur were shipped to the U.S. and converted to SPC (by reaction with 5 wt% organic modifiers) for use in this study. A phosphogypsum sand waste generated in Kazakhstan during the purification of phosphate fertilizer was selected for treatment. Waste loading of 40 wt% were easily achieved. Waste form performance testing included compressive strength, water immersion, and Accelerated Leach Testing. 14 refs., 7 figs., 6 tabs.
Date: August 1997
Creator: Yim, Sung Paal; Kalb, P. D. & Milian, L. W.
Partner: UNT Libraries Government Documents Department


Description: This report describes a DOE Accelerated Site Technology Deployment project being conducted at Brookhaven National Laboratory to deploy innovative, radiological, in situ analytical techniques. The technologies are being deployed in support of efforts to characterize the Brookhaven Graphite Research Reactor (BGRR) facility, which is currently undergoing decontamination and decommissioning. This report focuses on the deployment of the Canberra Industries In Situ Object Counting System (ISOCS) and assesses its data comparability to baseline methods of sampling and laboratory analysis. The battery-operated, field deployable gamma spectrometer provides traditional spectra of counts as a function of gamma energy. The spectra are then converted to radionuclide concentration by applying innovative efficiency calculations using monte carlo statistical methods and pre-defined geometry templates in the analysis software. Measurement of gamma emitting radionuclides has been accomplished during characterization of several BGRR components including the Pile Fan Sump, Above Ground Ducts, contaminated cooling fans, and graphite pile internals. Cs-137 is the predominant gamma-emitting radionuclide identified, with smaller quantities of Co-60 and Am-241 detected. The Project used the Multi-Agency Radiation Survey and Site Investigation Manual guidance and the Data Quality Objectives process to provide direction for survey planning and data quality assessment. Analytical results have been used to calculate data quality indicators (DQI) for the ISOCS measurements. Among the DQIs assessed in the report are sensitivity, accuracy, precision, bias, and minimum detectable concentration. The assessment of the in situ data quality using the DQIs demonstrates that the ISOCS data quality can be comparable to definitive level laboratory analysis when the field instrument is supported by an appropriate Quality Assurance Project Plan. A discussion of the results obtained by ISOCS analysis of objects that could not be analyzed readily by conventional methods demonstrates a powerful application of the instrument. In conclusion, a comparison of costs associated with the analysis on ...
Date: March 1, 2001
Partner: UNT Libraries Government Documents Department


Description: Thermokinetic mixing was investigated as an alternative processing method for polyethylene microencapsulation, a technology well demonstrated for treatment of hazardous, low-level radioactive and low-level mixed wastes. Polyethylene encapsulation by extrusion has been previously shown to be applicable to a wide range of waste types but often pretreatment of the wastes is necessary due to process limitations regarding the maximum waste moisture content and particle size distribution. Development testing was conducted with kinetic mixing in order to demonstrate technology viability and show improved process applicability in these areas. Testing to establish process capabilities and relevant operating parameters was performed with waste surrogates including an aqueous evaporator concentrate and soil. Using a pilot-scale kinetic mixer which was installed and modified for this program, the maximum waste moisture content and particle size was determined. Following process development with surrogate wastes, the technology was successfully demonstrated at BNL using actual mixed waste.
Date: November 1, 1997
Partner: UNT Libraries Government Documents Department

Deployment of Smart 3D Subsurface Contaminant Characterization at the Brookhaven Graphite Research Reactor

Description: The Brookhaven Graphite Research Reactor (BGRR) Historical Site Assessment (BNL 1999) identified contamination inside the Below Grade Ducts (BGD) resulting from the deposition of fission and activation products from the pile on the inner carbon steel liner during reactor operations. Due to partial flooding of the BGD since shutdown, some of this contamination may have leaked out of the ducts into the surrounding soils. The baseline remediation plan for cleanup of contaminated soils beneath the BGD involves complete removal of the ducts, followed by surveying the underlying and surrounding soils, then removing soil that has been contaminated above cleanup goals. Alternatively, if soil contamination around and beneath the BGD is either non-existent/minimal (below cleanup goals) or is very localized and can be ''surgically removed'' at a reasonable cost, the BGD can be decontaminated and left in place. The focus of this Department of Energy Accelerated Site Technology Deployment (DOE ASTD) project was to determine the extent (location, type, and level) of soil contamination surrounding the BGD and to present this data to the stakeholders as part of the Engineering Evaluation/Cost Analysis (EE/CA) process. A suite of innovative characterization tools was used to complete the characterization of the soil surrounding the BGD in a cost-effective and timely fashion and in a manner acceptable to the stakeholders. The tools consisted of a tracer gas leak detection system that was used to define the gaseous leak paths out of the BGD and guide soil characterization studies, a small-footprint Geoprobe to reach areas surrounding the BGD that were difficult to access, two novel, field-deployed, radiological analysis systems (ISOCS and BetaScint) and a three-dimensional (3D) visualization system to facilitate data analysis/interpretation. All of the technologies performed as well or better than expected and the characterization could not have been completed in the same time or ...
Date: February 26, 2002
Creator: Sullivan, T.; Heiser, J.; Kalb, P.; Milian, L.; Newson, C.; Lilimpakas, M. et al.
Partner: UNT Libraries Government Documents Department