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At least 19 records

Assessment the leaching characteristics and long-term leaching behavior of some radionuclides from synthesized zeolite cement matrix

Highlights: • Synthesis and characterization of zeolite cement synthesized from fly ash • Leaching tests were used to assess the release rate of {sup 85}Sr and {sup 60}Co radionuclides. • Simple mathematical models were used to detect leaching mechanisms. • Long-term leaching behavior of {sup 85}Sr and {sup 60}Co from cementitious matrix was assessed. The development of cementitious materials remains a vital goal to produce valuable products with good mechanical, physical and chemical properties suitable for the safe disposal of concentrated radionuclides resulted from the treatment of contaminated solutions. In this paper, zeolite cement with good properties was laboratory synthesized from industrial by-products fly ash and characterized using various characterization techniques. The leaching characteristics of strontium and cobalt radionuclides from the synthesized zeolite cement were scrutinized conforming with the standard leaching methodology of International Atomic Energy Authority (IAEA). A mechanical strength assessment was executed to characterize the extent of immobilization process of the solidified matrices. The cumulative leaching fraction (φ) of the two studied radionuclides was found to be less than 5% in all examined conditions, which implies the applicability of the IAEA-recommended methodology for estimating the diffusion coefficient. The experimental leaching data were regressed nonlinearly to various mathematical kinetic models to assess the controlling leaching mechanism and to determine the leaching parameters. The regression results indicated that strontium ({sup 85}Sr) and cobalt ({sup 60}Co) leaching resulted from two succeeding mechanisms: as first order kinetic reaction, and then diffusion. The calculated values of leachability indices signify that the performance of each of the studied matrices is within an acceptable range. A simplified mathematical model, rooted in the first order reaction and diffusion mechanisms, was simulated to predict the radionuclides leaching rates from zeolite cement matrices. By comparing the synthesized zeolite cement with other cementitious materials, it can be concluded that the synthesized material can be classified as an efficient material suitable to immobilize {sup 85}Sr and {sup 60}Co from radioactive wastes. The acquired findings demonstrated that the studied immobilized waste matrices have acceptable mechanical effectiveness.

36 MATERIALS SCIENCE↗

Deconsolidation and Leach Burn Leach of Seven As Irradiated AGR 5/6/7 TRISO Fuel Compacts from Capsules 2, 3, 4, and 5

Seven as-irradiated Advanced Gas Reactor (AGR) 5/6/7 compacts underwent destructive post-irradiation examination via deconsolidation-leach-burn leach at Idaho National Laboratory (INL). The selection of the compacts extended the upper and lower limits of time-average volume-average (TAVA) temperature for compacts that had gone through deconsolidation-leach-burn leach so far. The measured inventories of fission products and actinides in the compact matrix and outer pyrolytic carbon were reported. Results indicated unexpectedly higher rates of fuel kernel leaching compared to compacts from AGR-1 and AGR-2. These failure rates were attributed to damage during post-irradiation sample handling, rather than irradiation itself. AGR-5/6/7 compacts have little or no matrix coverage for some particles at the top and bottom ends of cylindrical fuel compacts, making them more fragile. Sixty particles were randomly sampled from each compact, and the gamma results were reported. Three SiC shells from were identified, one of which showed signs of chemical attack in the high-irradiation temperature compact.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Leaching Model of Radionuclides in Metal-Organic Framework Particles

Metal-organic frameworks (MOFs) have been used to sequester radionuclides and seal them inside of porous scaffolds using postsynthetic modification procedures. Experiments show that certain Zr-MOF with different capping linkers significantly affects the radionuclide release kinetics. In this work, we developed a leaching model of radionuclides in Zr-MOF particles. The model assumes that uranyl species occupy two energetically favored sites: the metal node and the MOF pores. For a given overall concentration of uranyl species, the partitions of uranyl species at the metal nodes and within the pores are determined by their chemical potentials. The model also considers the effect of particle surface and concentration on chemical potentials and diffusivity. The effects of spatial and structural dependent chemical potentials and diffusivity as well as particle sizes on leaching kinetics are investigated with the model. Predicted and measured uranyl leaching kinetics in Zr-MOF particles under batch experiments are compared. The results demonstrate the model’s capability for exploring the mechanisms of leaching and provide guidance for material design.

Metal-Organic Framework, Diffusion, uranyl, Leachi↗

ORNL Analysis of Leach-Burn-Leach Round-Robin Test Samples

An international round-robin test to examine the consistency in leach-burn-leach (LBL) analysis of tristructural-isotropic- (TRISO-) coated particle fuel was conducted by three research organizations from the Generation IV International Forum member countries of the People’s Republic of China, the Republic of Korea, and the United States of America. Two sets of round-robin test samples were exchanged for analysis. One set of samples consisted of a series of nonuranium-bearing, TRISO-coated zirconium dioxide particles seeded with up to four depleted uranium-bearing, TRISO-coated uranium dioxide (UO 2 ) particles, which had intentionally damaged coating layers to simulate either particles with either exposed-kernel defects (i.e., particles with a cracked TRISO coating that should be detected during preburn leaching) or particles with silicon carbide (SiC) defects (i.e., particles with an intact pyrocarbon coating and a hole in the SiC layer that should be detected during postburn leaching). These simulated samples also contained added powder with known quantities of impurities from a coal standard. The other sample set consisted of representative sublots of UO 2 -TRISO particles fabricated in a production-scale coater, except they all contained depleted uranium instead of enriched uranium. In this report, the methodology used at Oak Ridge National Laboratory to conduct LBL analysis of the round-robin samples is presented, and the general results are summarized.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Summary of Leach-Burn-Leach Round-Robin Test Results

Tristructural isotropic (TRISO) coated particle fuel is of interest to multiple member states associated with the Generation IV International Forum (GIF). Qualification and acceptance testing of TRISO fuel includes the determination of particle defect fractions and impurities in the as-fabricated TRISO fuel particle and/or composited fuel form, which are typically determined using burn-leach (BL) or leach-burn-leach (LBL) analysis methods. A round-robin test focusing on LBL analysis was undertaken by the GIF Very High Temperature Reactor System Fuel and Fuel Cycle Project Management Board. Participating in this LBL round-robin test were research staff from the Institute of Nuclear and New Energy Technology (INET) in the People’s Republic of China, the Korean Atomic Energy Research Institute (KAERI) in the Republic of Korea, and Oak Ridge National Laboratory (ORNL) in the United States of America. The motivation of this LBL benchmarking exercise was to explore consistency in results generated by LBL and to elucidate the potential influence of variations in the procedures used by the participating members on the accurate determination of the measured fuel properties.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Leaching behavior of microtektite glass compositions in sea water and the effect of precipitation on glass leaching

The present study attempts to account for the slow corrosion rates of microtektite glass in nature by comparing the leach rates of synthetic microtektite glass samples in deionized water and in sea-water, respectively. In order to obtain systematic data about leachant composition effects, leach tests were also carried out with synthetic leachant compositions enriched with respect to silica or depleted with respect to certain major components of sea-water (Mg, Ca).

Source record↗

Radial Deconsolidation and Leach-Burn-Leach of Eight As-Irradiated AGR-3/4 TRISO Fuel Compacts

Eight as-irradiated AGR-3/4 fuel compacts were subjected to destructive post-irradiation examination via radial-deconsolidation-leach-burn-leach (RDLBL) at INL. The RDLBL process deconsolidated the compacts in multiple, radial steps, followed by a final, single-step axial deconsolidation. The samples generated at each step were analyzed for isotopes of key fission products and actinides. After each deconsolidation step, the compact volume was assessed, and this was used to normalize the measured quantity of nuclides of interest to give a volumetric concentration as a function of radial position within the compact. The total inventories of measured fission products and actinides and the radial concentration profiles were compared among the eight compacts deconsolidated at INL and four other as-irradiated compacts examined at ORNL. The results were analyzed for the effects of irradiation temperature. These results will be used for comparisons with fission product transport models and as input from which fission product diffusivities can be calculated.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Radial Deconsolidation Leach-Burn-Leach of Five AGR-3/4 TRISO Fuel Compacts after Post-Irradiation Heating Tests

Five AGR-3/4 fuel compacts were previously heated in the Fuel Accident Condition Simulator (FACS) furnace. Three of these compacts were also reirradiated in the Neutron Radiography (NRAD) reactor before the FACS tests. One of these was heated to 1200°C, two were heated to 1400°C, one was heated to 1600°C, and one was held for a period of time at 1600 and 1700°C. After these FACS tests, the compacts were subjected to destructive post-irradiation examination (PIE) via radial-deconsolidation-leach-burn-leach (RDLBL) at INL. The RDLBL process deconsolidated the compacts in multiple radial steps, followed by a final, single-step axial deconsolidation. The samples generated at each step were analyzed for isotopes of key fission products and actinides. After each deconsolidation step, the compact volume was assessed, and this was used to normalize the measured quantities of nuclides of interest to give volumetric concentrations as a function of radial position within the compact. The total inventories of measured fission products and actinides and the radial concentration profiles were compared with their sibling compacts within the same capsule (similar irradiation conditions) that went through RDLBL in the as-irradiated state. These data will be used to refine the fission product transport models.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Radial Deconsolidation and Leach-Burn-Leach of AGR-3/4 Compact 1-4 and 10-4

The Advanced Gas Reactor (AGR) Fuel Development and Qualification Program third and fourth irradiation experiments (AGR-3/4), originally planned as separate tests, were combined in one test train for irradiation in the Advanced Test Reactor at Idaho National Laboratory (INL). The irradiation test began on December 14, 2011 and ended on April 12, 2014 (Collin 2016). The originally planned AGR-3 and AGR-4 irradiation experiments were both focused on obtaining data on fission product transport to support the improvement of modeling. The AGR-3 experimental plan was focused on gaseous and metallic fission product release from the kernels and diffusion in the coatings during irradiation and postirradiation safety testing. The AGR-4 experimental plan was focused on diffusivities and sorptivities in the compact matrix and reactor graphite (Petti et al. 2005). These two goals were combined in the AGR-3/4 irradiation, which consisted of twelve independently monitored capsules that each contained four AGR-3/4 compacts in a single stack surrounded by an inner ring of matrix or graphite and an outer ring of graphite. There were two capsule types: a standard capsule and a “fuel body”, in which the outer graphite ring included a floor and cap that fully enclosed the fuel (Stempien et al. 2018a). The fuel body design supported post-irradiation safety testing of the intact fuel and ring assembly to provide data on fission product transport and release from matrix and graphite at accident temperatures (Demkowicz 2017).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Radial Deconsolidation and Leach-Burn-Leach of AGR-3/4 Compacts 8-4 and 7-4

The Advanced Gas Reactor (AGR) Fuel Development and Qualification Program’s third and fourth irradiation experiments (AGR-3/4), originally planned as separate tests, were combined into one test train for irradiation in the Advanced Test Reactor at Idaho National Laboratory (INL). The irradiation test began on December 14, 2011, and ended on April 12, 2014 (Collin 2016). The originally planned AGR-3 and AGR-4 irradiation experiments were both to be focused on obtaining fission product transport data to support improvements in modeling. The AGR-3 experimental plan was focused on gaseous and metallic fission product release from the kernels and diffusion in the coatings during irradiation and postirradiation safety testing. The AGR-4 experimental plan was focused on diffusivities and sorptivities in the compact matrix and reactor graphite (Petti et al. 2005). These goals were combined in the AGR-3/4 irradiation experiment, which consisted of twelve independently monitored capsules that each contained four AGR-3/4 compacts in a single stack surrounded by an inner ring of matrix or graphite and an outer ring of graphite. There were two capsule types: a standard capsule and a fuel body, in which the outer graphite ring included a floor and cap to fully enclose the fuel (Stempien et al. 2018a). The fuel body design supported post-irradiation safety testing of the intact fuel and ring assembly to obtain data on fission product transport and release from matrix and graphite at accident temperatures (Demkowicz 2017).

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Radial Deconsolidation and Leach-Burn-Leach of AGR-3/4 Compacts 1-3, 4-3, 10-1, and 10-2

The Advanced Gas Reactor (AGR) Fuel Development and Qualification Program’s third and fourth irradiation experiments (AGR-3/4), originally planned as separate tests, were combined into one test train for irradiation in the Advanced Test Reactor at Idaho National Laboratory (INL). The irradiation test began on December 14, 2011 and ended on April 12, 2014 (Collin 2016). The originally planned AGR-3 and AGR-4 irradiation experiments were both focused on obtaining data on fission product transport to support modeling improvement. The AGR-3 experimental plan was focused on gaseous and metallic fission product release from the kernels and diffusion in the coatings during irradiation and post-irradiation safety testing. The AGR-4 experimental plan was focused on diffusivities and sorptivities in the compact matrix and reactor graphite (Petti et al. 2005). These two goals were combined in the AGR-3/4 irradiation, which consisted of twelve independently monitored capsules that each contained four AGR-3/4 compacts in a single stack surrounded by an inner ring of matrix or graphite and an outer ring of graphite. There were two capsule types: a standard capsule and a fuel body in which the outer graphite ring included a floor and cap that fully enclosed the fuel (Stempien et al. 2018a). The fuel body design supported post-irradiation safety testing of the intact fuel and ring assembly to provide data on fission product transport and release from matrix and graphite at accident temperatures (Demkowicz 2017)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Leaching Kinetics of Rare Earth Elements from Fire Clay Seam Coal

Recovery of rare earth elements (REEs) from coal samples collected from the Fire Clay coal seam using diluted mineral acid solutions was investigated. The initial processing step was coal recovery using conventional froth flotation which concentrated the REEs in tailing material resulting in an upgrade to values around 700 ppm on a dry whole mass basis. Leaching experiments were performed on the flotation tailings material using a 1.2 M sulfuric acid solution adjusted to a temperature of 75 °C to study the extractability of REEs from coal material. The effect of particle size, leaching time, leaching temperature, and solid concentration on REE leaching recovery were evaluated. The kinetic data obtained from leaching over a range of temperatures suggested that the leaching process follows the shrinking core model with possibly a mixed control mechanism that may be a result of several heterogenous materials leaching simultaneously. Leaching recovery increased rapidly at the beginning of the reaction then slowed as the system reached equilibrium. The apparent activation energy determined from test data obtained over a range of temperatures using 1 M sulfuric acid was 36 kJ/mol for the first 20 min of reaction time and 27 kJ/mol for the leaching period between 20 and 120 min. The leaching of light REEs during the initial stage was determined to be driven by a chemical reaction, followed by the formation of a product layer, which required lower activation energy in the later stage of leaching. In regards to the heavy REEs, the major mechanism for leaching is desorption and the product layer formation does not affect the heavy REEs significantly.

58 GEOSCIENCES↗

Development of an In-Situ Leaching Technology for Extracting Residual Uranium from Remediated Soil - 20099

Site-specific chemical solutions for extracting uranium were developed and evaluated for treating previously remediated soil at a former thorium mill tailings site, known as the Former Rare Earths Facility (REF), in West Chicago, Illinois. Prior remediation efforts had resulted in residual sand and gravel aggregate that met the soil cleanup standards. The target soil contains residual levels of uranium, which continues to leach into the site groundwater at levels exceeding groundwater protection standards (GWPS). A series of bench-scale tests were conducted to evaluate the efficacy and viability of in-situ leaching (ISL) technology to treat the target soil for the purposes of attaining uranium GWPS at the REF. Specific objectives of the bench-scale tests entailed identification and selection of optimal leaching, quantification of the extent and rate of uranium released as a function of chemical composition, chemical concentrations, chemical residence times, and obtaining critical data to estimate treatment costs. A combination of sodium bicarbonate and sodium carbonate reagent was the most effective leaching solution. In general, leaching solutions containing a higher concentration of sodium carbonate demonstrated superior uranium leaching capabilities. Removal of 50% of the uranium mass from the soil matrix was adequate for achieving compliance with the site-specific GWPS. After six to seven pore volume flushes (PVFs), the uranium leaching effectiveness of all leaching solutions was similar. The amount of initial uranium removed with each subsequent PVF was minimal, suggesting limited solubility of the remaining mass of uranium. The effects of leaching duration were significant and persisted through at least the first five consecutive PVFs. Leaching of uranium also resulted in leaching of several non-uranium constituents, many of which exceeded applicable National Pollutant Discharge Elimination System (NPDES) standards. Given historical operations and waste disposal practices at the site, leaching of non-uranium constituents was expected. Hydrochloric acid was used to stabilize treated soil. Savings of approximately $148 million in direct and indirect remediation costs are expected with an ISL alternative compared to the excavation and landfill disposal remediation option. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Automation of Plot Generation for Strategic Petroleum Reserve Cavern Leaching Monitoring

Monitoring cavern leaching after each calendar year of oil sales is necessary to support cavern stability efforts and long-term availability for oil drawdowns in the U.S. Strategic Petroleum Reserve. Modeling results from the SANSMIC code and recent sonars are compared to show projected changes in the cavern’s geometry due to leaching from raw-water injections. This report aims to give background on the importance of monitoring cavern leaching and provide a detailed explanation of the process used to create the leaching plots used to monitor cavern leaching. In the past, generating leaching plots for each cavern in a given leaching year was done manually, and every cavern had to be processed individually. A Python script, compatible with Earth Volumetric Studio, was created to automate most of the process. The script makes a total of 26 plots per cavern to show leaching history, axisymmetric representation of leaching, and SANSMIC modeling of future leaching. The current run time for the script is one hour, replacing 40-50 hours of the monitoring cavern leaching process.

02 PETROLEUM↗