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Evaluation of Observed and Modelled Aerosol Lifetimes Using Radioactive Tracers of Opportunity and an Ensemble of 19 Global Models

Aerosols have important impacts on air quality and climate, but the processes affecting their removal from the atmosphere are not fully understood and are poorly constrained by observations. This makes modelled aerosol lifetimes uncertain. In this study, we make use of an observational constraint on aerosol lifetimes provided by radionuclide measurements and investigate the causes of differences within a set of global models. During the Fukushima Dai-Ichi nuclear power plant accident of March 2011, the radioactive isotopes cesium-137 (Cs-137) and xenon-133 (Xe-133) were released in large quantities. Cesium attached to particles in the ambient air, approximately according to their available aerosol surface area. Cs-137 size distribution measurements taken close to the power plant suggested that accumulation mode (AM) sulfate aerosols were the main carriers of cesium. Hence, Cs-137 can be used as a proxy tracer for the AM sulfate aerosol's fate in the atmosphere. In contrast, the noble gas Xe-133 behaves almost like a passive transport tracer. Global surface measurements of the two radioactive isotopes taken over several months after the release allow the derivation of a lifetime of the carrier aerosol. We compare this to the lifetimes simulated by 19 different atmospheric transport models initialized with identical emissions of Cs-137that were assigned to an aerosol tracer with each model's default properties of AM sulfate, and Xe-133 emissions that were assigned to a passive tracer. We investigate to what extent the modelled sulfate tracer can reproduce the measurements, especially with respect to the observed loss of aerosol mass with time. Modelled Cs-137and Xe-133 concentrations sampled at the same location and times as station measurements allow a direct comparison between measured and modelled aerosol lifetime. The e-folding lifetime e, calculated from station measurement data taken between 2 and 9 weeks after the start of the emissions, is 14.3 days (95% confidence interval 13.1-15.7 days). The equivalent modelled e lifetimes have a large spread, varying between 4.8 and 26.7 days with a model median of 9.42.3 days, indicating too fast a removal in most models. Because sufficient measurement data were only available from about 2 weeks after the release, the estimated lifetimes apply to aerosols that have undergone long-range transport, i.e. not for freshly emitted aerosol. However, modelled instantaneous lifetimes show that the initial removal in the first 2 weeks was quicker (lifetimes between 1 and 5 days) due to the emissions occurring at low altitudes and co-location of the fresh plume with strong precipitation. Deviations between measured and modelled aerosol lifetimes are largest for the northernmost stations and at later time periods, suggesting that models do not transport enough of the aerosol towards the Arctic. The models underestimate passive tracer (Xe-133) concentrations in the Arctic as well but to a smaller extent than for the aerosol (Cs-137) tracer. This indicates that in addition to too fast an aerosol removal in the models, errors in simulated atmospheric transport towards the Arctic in most models also contribute to the underestimation of the Arctic aerosol concentrations.

Radioactive isotopes↗

Radioactivity Calculator for Research and Test Reactor Neutron-Activated Materials

The Idaho National Laboratory Nuclear Science User Facilities program is proposing to launch a new online expert system that will assist users in planning experiments and writing proposals. The Combined Materials Experimentation Toolkit (CoMET) will include two nuclear calculators. The first of these, the Neutron Damage Calculator, will assist users in selecting reactor positions in order to obtain desired material damage in Damage Per Atom (DPA) and provide the required irradiation time to reach the damage levels. The second, the Radioactivity Calculator, will estimate the post-irradiation radioactivity levels of sample materials, which will inform technical staff of examination facility requirements and any potential scheduling delays. Both of these calculators were designed to simplify the information needed from users in order to properly plan and execute awarded proposals. This paper presents the primary purpose and methodologies implemented by these two calculators.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Digital Autoradiography as a novel complementary technique for the investigation of radioactive contamination in nuclear facilities under dismantlement

The detection (location and quantification) of nuclear facilities to be dismantled possible contamination with low-range particles emitters ({sup 3}H, other low-energy β emitters, a emitters) remains a tedious and expensive task. Indeed, usual remote counters show a too low sensitivity to these non-penetrating radiations, while conventional wipe tests are irrelevant for fixed radioactivity evaluation. The only method to accurately measure activity levels consists in sampling and running advanced laboratory analyses (spectroscopy, liquid scintillation counting, pyrolysis...). Such measurements generally induce sample preparation, waste production (destructive analyses, solvents), nuclear material transportation, long durations, and significant labor mobilization. Therefore, the search for the limitation of their number and cost easily conflicts with the necessity to perform a dense screening for sampling (to maximize the representativeness of the samples), in installations of thousands of square meters (floors, wells, ceilings), plus furniture, pipes, and other wastes. To overcome this contradiction, Digital Autoradiography (D. A.) was re-routed from bio molecular research to radiological mapping of nuclear installations under dismantling and to waste and sample analysis. After in-situ exposure to the possibly-contaminated areas to investigate, commercial reusable radiosensitive phosphor screens (of a few 100 cm{sup 2}) were scanned in the proper laboratory device and sharp quantitative images of the radioactivity could be obtained. The implementation of geostatistical tools in the data processing software enabled the exhaustive characterization of concrete floors at a rate of 2 weeks / 100 m{sup 2}, at lowest costs. Various samples such as drilled cores, or tank and wood pieces, were also successfully evaluated with this method, for decisive results. Thanks to the accurate location of potential contamination spots, this approach ensures relevant and representative sampling for further laboratory analyses and should be inserted in the range of common tools used in dismantling. (authors)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Radioactivity and neutron damage calculators for research and test reactor neutron-activated materials - 25652

The Idaho National Laboratory Nuclear Science User Facilities program is proposing to launch a new online expert system that will assist users in planning experiments and writing proposals. The Combined Materials Experimentation Toolkit (CoMET) will include two nuclear calculators. The first of these, the Neutron Damage Calculator, will assist users in selecting reactor positions in order to obtain desired material damage in Damage Per Atom (DPA) and provide the required irradiation time to reach the damage levels. The second, the Radioactivity Calculator, will estimate the post-irradiation radioactivity levels of sample materials, which will inform technical staff of examination facility requirements and any potential scheduling delays. Both of these calculators were designed to simplify the information needed from users in order to properly plan and execute awarded proposals. This paper presents the primary purpose and methodologies implemented by these two calculators. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

The Polymers for Liquid Radioactive Waste Solidification: a Lost Chapter in the History of Engineering or a Step Forward? - 13529

Ideas on the application of polymers for the liquid radioactive waste immobilization go a way back, and the first studies in the area were published 30-40 years ago. One should admit that regardless of the fairly large number of publications appeared in the past years currently the interest in this work came down greatly. It was the successful assimilation and worldwide implementation of the LRW cementation technology caused a slump in the interest in polymers. But today it's safe to say that the situation slowly changes, particularly due to the market appearance of the high-tech polymers manufactured by Nochar Company, and unique properties of these polymers gradually raise the demand in various countries. The results of multiple experiments performed with the simulated solutions have passed the comprehensive tests with actual waste. The economic effect from the implementation of the new technology is defined by the volume reduction of waste coming onto the repository, by the decline in the cost of transportation and of the repository construction on account of cutting down the construction volume. Interesting results have been obtained during the search for the technical decisions that would allow using the polymer materials in the processing technology of the industrial toxic waste. One more promising area of the possible application of polymers should be pointed out. It is the application of polymer materials as the assets for the emergency damage control when the advantages of the polymers become obvious. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Preliminary safety evaluation of an aircraft impact on a near-surface radioactive waste repository

The aircraft impact accident has become very significant in the design of a nuclear facilities, particularly, after the tragic September 2001 event, that raised the public concern about the potential damaging effects that the impact of a large civilian airplane could bring in safety relevant structures. The aim of this study is therefore to preliminarily evaluate the global response and the structural effects induced by the impact of a military or commercial airplane (actually considered as a 'beyond design basis' event) into a near surface radioactive waste (RWs) disposal facility. The safety evaluation was carried out according to the International safety and design guidelines and in agreement with the stress tests requirements for the security track. To achieve the purpose, a lay out and a scheme of a possible near surface repository, like for example those of the El Cabril one, were taken into account. In order to preliminarily perform a reliable analysis of such a large-scale structure and to determine the structural effects induced by such a types of impulsive loads, a realistic, but still operable, numerical model with suitable materials characteristics was implemented by means of FEM codes. In the carried out structural analyses, the RWs repository was considered a 'robust' target, due to its thicker walls and main constitutive materials (steel and reinforced concrete). In addition to adequately represent the dynamic response of repository under crashing, relevant physical phenomena (i.e. penetration, spalling, etc.) were simulated and analysed. The preliminary assessment of the effects induced by the dynamic/impulsive loads allowed generally to verify the residual strength capability of the repository considered. The obtained preliminary results highlighted a remarkable potential to withstand the impact of military/large commercial aircraft, even in presence of ongoing concrete progressive failure (some penetration and spalling of the concrete wall) of the impacted area. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Current status and performance assessment for the Techa cascade of reservoirs - liquid radioactive waste storage facility

The Techa cascade of water reservoirs is the world's largest open storage facility for liquid low-level radioactive waste. Its capacity is about 360 mln. m{sup 3}, it occupies an area of more than 65 km{sup 2}, the total activity accumulated in the water and sediments is about 6.10{sup 15} Bq. The major challenge facing the Techa cascade is virtually uncontrollable water level changes. The water level rise can cause significant pollution of the environment. From the late 1990's onwards, the issue of the Techa cascade safety assurance is considered to be one of the major challenges pertaining to nuclear legacy for 'Mayak' and Russia as a whole. Unlike other industrial water reservoirs the Techa cascade liquidation is estimated as highly unrealistic. The main objectives of the paper are: - brief results summary of the practical works on safety improvement at the Techa cascade carried out over the past decade; - introduction the works on the Techa cascade performance assessment; - determination of the existing risks and strategic areas for solving the problem. (authors)

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Determination of Erosion/Corrosion Rates in Hanford Tank Farms Radioactive Waste Transfer System Pipelines

The twenty-eight double-shell underground radioactive waste storage tanks at the U. S. Department of Energy’s Hanford Site near Richland, WA are interconnected by the Waste Transfer System network of buried steel encased pipelines and pipe jumpers in below-grade pits. The pipeline material is stainless steel or carbon steel in 51 mm to 152 mm (2 in. to 6 in.) sizes. The pipelines carry slurries ranging up to 20 volume percent solids and supernatants with less than one volume percent solids at velocities necessary to prevent settling. The pipelines, installed between 1976 and 2011, were originally intended to last until the 2028 completion of the double-shell tank storage mission. The mission has been subsequently extended. In 2010 the Tank Operating Contractor began a systematic evaluation of the Waste Transfer System pipeline conditions applying guidelines from API 579-1/ASME FFS-1 (2007), Fitness-For-Service. Between 2010 and 2014 Fitness-for-Service examinations of the Waste Transfer System pipeline materials, sizes, and components were completed. In parallel, waste throughput histories were prepared allowing side-by-side pipeline wall thinning rate comparisons between carbon and stainless steel, slurries and supernatants and throughput volumes. The work showed that for transfer volumes up to 6.1E+05 m 3 (161 million gallons), the highest throughput of any pipeline segment examined, there has been no detectable wall thinning in either stainless or carbon steel pipeline material regardless of waste fluid characteristics or throughput. The paper describes the field and laboratory evaluation methods used for the Fitness-for-Service examinations, the results of the examinations, and the data reduction methodologies used to support Hanford Waste Transfer System pipeline wall thinning conclusions.

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Environmental Effects of Cavitation Technology for Radioactive Waste Management

Results from studies of the removal from storage and solidification of low- and intermediate-level liquid radioactive waste in inorganic binders (cementation) are presented. Cavitation technology for recycling radiochemical wastes from nuclear power plant decommissioning increases the extraction throughput and strength of the cement compound.

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Effect of supplementary cementitious materials on the degradation of cement-based barriers in radioactive waste repository: A case study in Korea

This study focuses on investigating the chemical degradation characteristics of cementitious barriers used in low- and intermediate-level radioactive waste repository by reactive transport modeling. The impact of the blending with supplementary cementitious materials (SCMs) in the barriers on the chemical degradation was evaluated to find the optimum barrier design. A number of different barrier designs were examined by replacing ordinary Portland cement (OPC) by SCMs (i.e., fly ash, silica fume, and blast-furnace slag). The simulation results showed that silica fume blended barrier has better durability against chemical degradation by rainwater compared to fly ash or blast-furnace slag blended barriers. In addition, the chemical durability of silica fume-based barrier increased with increasing replacement level up to about 20 %. It seems that the amount of formed calcium silicate hydrate (CSH) in the initial cement-based barrier highly affects the overall chemical durability. The newly developed reactive transport model demonstrated its capability for understanding the barrier performance and investigating the optimal design of the barrier system.

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Development of characterization protocol for mixed liquid radioactive waste classification

Mixed liquid organic waste generated from health-care and research activities containing tritium, carbon-14, and other radionuclides posed specific challenges in its management. Often, these wastes become legacy waste in many nuclear facilities and being considered as ‘problematic’ waste. One of the most important recommendations made by IAEA is to perform multistage processes aiming at declassification of the waste. At this moment, approximately 3000 bottles of mixed liquid waste, with estimated volume of 6000 litres are currently stored at the National Radioactive Waste Management Centre, Malaysia and some have been stored for more than 25 years. The aim of this study is to develop a characterization protocol towards reclassification of these wastes. The characterization protocol entails waste identification, waste screening and segregation, and analytical radionuclides profiling using various analytical procedures including gross alpha/ gross beta, gamma spectrometry, and LSC method. The results obtained from the characterization protocol are used to establish criteria for speedy classification of the waste.

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The Belgian R and D feasibility programme on the geological disposal of high-level and long-lived radioactive waste

ONDRAF/NIRAS, the Belgian Agency for Radioactive Waste and Enriched Fissile Materials, considers geological disposal in poorly indurated clay as the reference solution for the long-term management of high-level waste (HLW) and intermediate and low level waste, long-lived (ILLW-LL). The disposal concept entails the post-conditioning of the waste in disposal packages and the subsequent disposal of these packages in an underground repository. The R and D feasibility programme on geological disposal aims at demonstrating, at a conceptual level, that the proposed disposal system can be constructed, operated and closed. (authors)

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Development of low-pH cements for immobilisation of intermediate level radioactive waste: achievements and challenges

Although cementation is a widely recognized solidification/ stabilization process for immobilisation of Intermediate Level Radioactive Waste (ILRW), the low resistance to hyper-alkaline pore waters compromises the effectiveness of the process when Portland Cement (PC) is employed. Moreover the manufacture of PC is responsible for significant CO{sub 2} emissions. In this context, low pH cements are environmentally more suitable and have emerged as a potential alternative for obtaining secure waste forms. This paper summarises the achievements on development of low-pH cements and the challenges of using these new materials for the ILRW immobilisation. The performance of waste forms is also discussed in terms of radionuclides release. Reactive magnesium oxide and magnesium phosphate cements are emphasised as they feature important advantages such as consumption of available constituents for controlling acid-base reactions, reduced permeability and higher density. Additionally, in order to identify new opportunities for study, the long-term modelling approach is also briefly discussed. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Vacuum arc with a distributed cathode spot as a plasma source for plasma separation of spent nuclear fuel and radioactive waste

Results from experimental studies of a vacuum arc with a distributed cathode spot on the heated cathode are presented. Such an arc can be used as a plasma source for plasma separation of spent nuclear fuel and radioactive waste. The experiments were performed with a gadolinium cathode, the properties of which are similar to those of an uranium arc cathode. The heat flux from the plasma to the cathode (and its volt equivalent) at discharge voltages of 4-15 V and discharge currents of 44-81 A, the radial distribution of the emission intensity of gadolinium atoms and singly charged ions in the arc channel at a voltage of 4.3 V, and the plasma electron temperature behind the anode were measured. The average charge of plasma ions at arc voltages of 3.5-8 V and a discharge current of 52 A and the average rate of gadolinium evaporation in the discharge were also determined.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Nevada National Security Site 2015 Waste Management Monitoring Report Area 3 and Area 5 Radioactive Waste Management Sites

Environmental monitoring data are collected at and around the Area 3 and Area 5 Radioactive Waste Management Sites (RWMSs) within the Nevada National Security Site (NNSS). These data include direct radiation exposure, as well as radiation from the air, groundwater, meteorology, and vadose zone. This report summarizes the 2015 environmental data to provide an overall evaluation of RWMS performance and to support environmental compliance and performance assessment (PA) activities. Some of these data (e.g., radiation exposure, air, and groundwater) are presented in other reports developed by National Security Technologies, LLC. Direct radiation monitoring data indicate exposure levels at the RWMSs are within the range of background levels measured at the NNSS. Slightly elevated exposure levels outside the Area 3 RWMS are attributed to nearby historical aboveground nuclear weapons tests. Air monitoring data show that tritium concentrations in water vapor and americium and plutonium concentrations in air particles are below Derived Concentration Standards for these radionuclides. Groundwater monitoring data indicate the groundwater in the uppermost aquifer beneath the Area 5 RWMS is not impacted by RWMS operations. Results of groundwater analysis from wells around the Area 5 RWMS were all below established investigation levels. Leachate samples collected from the leachate collection system at the mixed low-level waste cell were below established contaminant regulatory limits. During 2015, precipitation at the Area 3 RWMS was 0.9% above average, and precipitation at the Area 5 RWMS was 25% above average. Water balance measurements indicate that evapotranspiration from the vegetated weighing lysimeter dries the soil and prevents downward percolation of precipitation more effectively than evaporation as measured from the bare-soil weighing lysimeter. The 1.8 inches of precipitation in September reached the lowest sensors at 180 cm on the Cell 5S and 5N covers, however the sensors on the floor do not indicate any signs of the precipitation percolating thru the waste to the floor. Moisture from precipitation did not percolate below 150 centimeters (cm) (5 feet [ft]) in the vegetated final cover on the U-3ax/bl disposal unit at the Area 3 RWMS. A second remedial revegetation trial was done on the southern portion of the North Cover. In March 2015 it was determined that germination occurred on both the mulched and non-mulched treatments that were irrigated, but that no germination occurred on the non-irrigated treatments. By June the seedlings observed in March were gone, possibly grazed by rabbits which were observed inside the rabbit-proof fence. In August the entire area was sprayed with the herbicide glyphosate in an attempt to minimize weed seed production. During 2015, there was no drainage through 2.4 meters (8 ft) of soil as indicated from the Area 3 drainage lysimeters that received only natural precipitation. Thirty-one percent of the applied precipitation and irrigation drained from the bare-soil drainage lysimeter, which received 3 times the natural precipitation. All 2015 monitoring data indicate that the Area 3 and Area 5 RWMSs are performing within expectations of the model and parameter assumptions for the facilities’ PAs.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Waste Handling and Emplacement Options for Disposal of Radioactive Waste in Deep Boreholes.

Traditional methods cannot be used to handle and emplace radioactive wastes in boreholes up to 16,400 feet (5 km) deep for disposal. This paper describes three systems that can be used for handling and emplacing waste packages in deep borehole: (1) a 2011 reference design that is based on a previous study by Woodward–Clyde in 1983 in which waste packages are assembled into “strings” and lowered using drill pipe; (2) an updated version of the 2011 reference design; and (3) a new concept in which individual waste packages would be lowered to depth using a wireline. Emplacement on coiled tubing was also considered, but not developed in detail. The systems described here are currently designed for U.S. Department of Energy-owned high-level waste (HLW) including the Cesium- 137/Strontium-90 capsules from the Hanford Facility and bulk granular HLW from fuel processing in Idaho.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Study on Shielding Requirements for Radioactive Waste Transportation in a Mo-99 Production Plant - 13382

Brazil is currently planning to produce {sup 99}Mo from fission of low enriched uranium (LEU) targets. The planned end of irradiation activity of {sup 99}Mo is about 185 TBq (5 kCi) per week to meet the present domestic demand of {sup 99m}Tc generators. The radioactive wastes from the production plant will be transferred to a waste treatment facility at the same site. The total activity of the actinides, fission and activation products present in the wastes can be predicted based on the yields of fission and activation data for the irradiation conditions, such as composition and mass of uranium targets, irradiation time, neutron flux, production schedule, etc., which were in principle already established by the project management. The transportation of the wastes from the production plant to the treatment facility will be done by means of special shielded packages. An assessment of the shielding required for the packages has been done and the results are presented here, aiming at contributing to the design of the waste management facility for the {sup 99}Mo production plant. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Linking RESRAD-OFFSITE and HYDROGEOCHEM Model for Performance Assessment of Low-Level Radioactive Waste Disposal Facility - 13429

Performance assessments are crucial steps for the long-term radiological safety requirements of low-level waste (LLW) disposal facility. How much concentration of radionuclides released from the near-field to biosphere and what radiation exposure levels of an individual can influence on the satisfactory performance of the LLW disposal facility and safety disposal environment. Performance assessment methodology for the radioactive waste disposal consists of the reactive transport modeling of safety-concerned radionuclides released from the near-field to the far-field, and the potential exposure pathways and the movements of radionuclides through the geosphere, biosphere and man of which the accompanying dose. Therefore, the integration of hydrogeochemical transport model and dose assessment code, HYDROGEOCHEM code and RESRAD family of codes is imperative. The RESRAD family of codes such as RESRAD-OFFSITE computer code can evaluate the radiological dose and excess cancer risk to an individual who is exposed while located within or outside the area of initial (primary) contamination. The HYDROGEOCHEM is a 3-D numerical model of fluid flow, thermal, hydrologic transport, and biogeochemical kinetic and equilibrium reactions in saturated and unsaturated media. The HYDROGEOCHEM model can also simulate the crucial geochemical mechanism, such as the effect of redox processes on the adsorption/desorption, hydrogeochemical influences on concrete degradation, adsorption/desorption of radionuclides (i.e., surface complexation model) between solid and liquid phase in geochemically dynamic environments. To investigate the safety assessment of LLW disposal facility, linking RESRAD-OFFSITE and HYDROGEOCHEM model can provide detailed tools of confidence in the protectiveness of the human health and environmental impact for safety assessment of LLW disposal facility. (authors)

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