Low-level Waste Research Articles

Effects of Effluent Stream Composition and Competing Reactions Effect on Wastewater Nitrate Reduction in a Photoelectrochemical Device

More than 80% of nitrogen-contaminants are present in the form of nitrates in point sources of wastewater, including municipal wastewater effluents, ion-exchange brines, low-level nuclear wastes and in power generation. Wastewater nitrates represent an untapped source for the recovery of nutrients, value-added chemicals, and energy. Nitrates can be reduced to form ammonia, which can be used as a fertilizer or fuel, and nitrous oxide, which is a powerful oxidizer for the combustion and supercharging applications. Depending upon the source of the wastewater, the concentration of nitrates present in these streams can vary significantly. Ion-exchange brines and low-level nuclear wastes have large nitrate concentrations, on the order of > 0.1 M, whereas municipal and power generation effluents are more dilute (0.1 mM). However, the effect of varying contaminant concentrations and the competing redox reactions have not been quantified for these systems.In this study, a photoelectrochemical device is proposed to transform wastewater nitrates into ammonia, coupled with water oxidation. We expand on a previously developed numerical model to include the effects of the reacting nitrate species concentrations and the competing redox reactions on the solar-to-chemical efficiencies and nitrogen-removal rates. Notably, we implemented an equivalent circuit modeling approach to account for the influences of the competing reactions and the concentration-dependent mass-transfer limiting current densities. Model results predict that for a single light-absorber and a nitrate concentration of 100 mM, the optimal solar-to-chemical efficiency is 7% and the nitrogen recovery rate (as NH3) is 260 gN m-2 day-1. Oxygen reduction is more dominant as a competing reaction than hydrogen reduction at the cathode. However, this reduction is mass-transfer limited even while assuming an air-saturated (1 atm) device and therefore didn’t impact the performance significantly. Modeling results are complemented by experimental measurements of the effects of nitrate concentrations on the operating current densities and the rates of product formation with copper and platinum electrodes at the cathode and anode respectively.

Immobilization of Liquid Radioactive Waste In Cement

Immobilization of radioactive waste is required to comply with nuclear regulations and waste acceptance criteria in a repository, which require the waste to be solid or immobilized in solid form within a durable and resistant matrix . Cement is the most frequently used material for the immobilization of liquid, low-level waste, since it has many advantages, such as the ease of preparation at room temperature and the low cost. In this paper, we describe the characteristics of cement-water mixtures, homogenized in a drum using a vibration table as the mixing device. Common Portland cement was used as the immobilization matrix. The homogeneity of the mixtures is evaluated using cement dye in appropriate amounts. Initially, the distribution of the mineral dye was made by visual inspection. The batches were carried out with three different ways of feeding the components. Different results were obtained depending on the feeding methods employed.

Study of cesium sorption by a Brazilian bentonite

Engineered and natural barriers compose the disposal system of near surface repository to store low and intermediate level radioactive wastes. Waterproofing barriers are constituted of clays, such as the bentonite, in order to avoid or to limit the release of radionuclides to with consequences to the environment and humans. Characteristics such as high cation exchange capacity, high adsorption capacity and high sealing capacity, are taken into consideration for choosing this material. The migration of radionuclides through protection barriers can occur in a variety of ways, such as surface water infiltration, groundwater intrusion, among others. Diffusion is the process which governs the contaminant transport through soil barriers. Adsorption is one of the processes that could be considered in the diffusion mechanism, and sorption isotherms are obtained from values measured in the batch-adsorption experiments. Therefore, such experiments were carried out in order to estimate the cesium sorption by the bentonite. The quantitative analysis was performed using atomic absorption and the energy dispersive X-ray fluorescence spectrometry. With the purpose to calculate the true value of cesium sorption, a mass-balance was made considering all the steps of the batch experiment, and it was found a 6% loss in the whole process. The quantity of cesium sorbed by the bentonite was 66.7 mg.g-1. At the moment, eight additional experiments are being performed, using solutions with different cesium concentrations, leading to all the necessary data for the isotherm.

Brazilian clays for environmental solutions applied to radioactive waste management

Clays have been adopted in most nuclear waste producing countries as a key constituent in engineered barrier systems for final disposal facilities at all levels of radioactive wastes (LILW-SL, LILW-LL, and HLW). The following study presents a thorough characterization upon five Brazilian clay-rich deposits, mostly smectite bearing clays, aiming to evaluate their expected performance as barrier under the conditions associated to a Low and Intermediate Level Waste Repository; being the former a matter of national strategic interest. Samples coming from the Brazilian states of Paraná, Bahia, Paraíba, and Maranhão were treated and analyzed by means of X-Ray diffraction as main technique, and complemented by FTIR, LALLS, XRF, and SEM-EDS, in order to establish the mineralogical composition, particle size distribution, and chemical composition. Moreover, several standard clay treatments over the <1 μm size fraction were carried out to reveal information regarding layer charge, major interlayer cations, unit formula and other crystal features of smectite species present in a mineralogical assembly, aiming to provide information for the construction of a molecular model over which would be realistic to simulate the diffusion of radionuclides. Results obtained on 133Cs adsorption experiments indicate that mineralogical composition would probably be the single most influential factor controlling transport capacity of positively charged radionuclides in the current setup. The composition is especially expressed in terms of smectite contents, favoring montmorillonite rich materials containing majorly Na+ as compensating cation in interlayer position. All tested samples can be considered as suitable candidates to be used in the design of final destination storage for nuclear waste. Thus, efficiency on 133Cs adsorption trials also indicate that these materials could have potential uses as sorptive matrices (Sorbents) for water treatment of radionuclide polluted waters such as TENORM waste waters. However, these trends are yet to be contrasted against hydraulic conductivity measurements and swelling pressure in order to have a more comprehensive perspective of this clayey prospects as barrier enhanced layer; aligned to the multilayer barrier system approach for nuclear waste management.

Selection of steel fibers dosage in concrete for repository containers

The use of nuclear energy, as well as all human activity, generates wastes and these need to receive suitable treatments so that they don’t expose a risk to the public and the environment. Currently there is a project in Brazil whose objective is the implementation of a national repository for the final storage of low and intermediate level waste. The disposal of the radioactive waste is based on the concept of multiple barriers, in which packed wastes are conditioned in concrete containers, which are then placed in modules, which are closed and covered by natural materials. In this work, Steel Fiber Reinforced Concrete (SFRC) was studied as a substitute for the concrete with conventional steel reinforcement in the production of containers. Compressive and tensile strength tests were performed, as well as characterization and evaluation of steel fibers. 48 specimens of concrete were prepared with two types of fibers (A and C) and tested. The best results were obtained with the addition of 1.5% vol. of type A fibers. Through the carbon and sulfur quantification test it was possible to conclude the steel used in the fibers’ manufacture was low carbon. It was also possible to verify, using the folding test, the material used served the parameters of quality. This research project was supported by the Centro de Desenvolvimento da Tecnologia Nuclear (CDTN), the Comissão Nacional de Energia Nuclear (CNEN) and the Fundação de Amparo à Pesquisa do Estado de Minas Gerais (FAPEMIG).

Microbial Degradation of Citric Acid in Low Level Radioactive Waste Disposal: Impact on Biomineralization Reactions

Organic complexants are present in some radioactive wastes and can challenge waste disposal as they may enhance subsurface mobility of radionuclides and contaminant species via chelation. The principal sources of organic complexing agents in low level radioactive wastes (LLW) originate from chemical decontamination activities. Polycarboxylic organic decontaminants such as citric and oxalic acid are of interest as currently there is a paucity of data on their biodegradation at high pH and under disposal conditions. This work explores the biogeochemical fate of citric acid, a model decontaminant, under high pH anaerobic conditions relevant to disposal of LLW in cementitious disposal environments. Anaerobic microcosm experiments were set up, using a high pH adapted microbial inoculum from a well characterized environmental site, to explore biodegradation of citrate under representative repository conditions. Experiments were initiated at three different pH values (10, 11, and 12) and citrate was supplied as the electron donor and carbon source, under fermentative, nitrate-, Fe(III)- and sulfate- reducing conditions. Results showed that citrate was oxidized using nitrate or Fe(III) as the electron acceptor at > pH 11. Citrate was fully degraded and removed from solution in the nitrate reducing system at pH 10 and pH 11. Here, the microcosm pH decreased as protons were generated during citrate oxidation. In the Fe(III)-reducing systems, the citrate removal rate was slower than in the nitrate reducing systems. This was presumably as Fe(III)-reduction consumes fewer moles of citrate than nitrate reduction for the same molar concentrations of electron acceptor. The pH did not change significantly in the Fe(III)-reducing systems. Sulfate reduction only occurred in a single microcosm at pH 10. Here, citrate was fully removed from solution, alongside ingrowth of acetate and formate, likely fermentation products. The acetate and lactate were subsequently used as electron donors during sulfate-reduction and there was an associated decrease in solution pH. Interestingly, in the Fe(III) reducing experiments, Fe(II) ingrowth was observed at pH values recorded up to 11.7. Here, TEM analysis of the resultant solid Fe-phase indicated that nanocrystalline magnetite formed as an end product of Fe(III)-reduction under these extreme conditions. PCR-based high-throughput 16S rRNA gene sequencing revealed that bacteria capable of nitrate Fe(III) and sulfate reduction became enriched in the relevant, biologically active systems. In addition, some fermentative organisms were identified in the Fe(III)- and sulfate-reducing systems. The microbial communities present were consistent with expectations based on the geochemical data. These results are important to improve long-term environmental safety case development for cementitious LLW waste disposal.

Liquid Low-Level Radioactive Waste Treatment Using an Electrodialysis Process.

In this work, the possibility of using electrodialysis for the treatment of liquid low-level radioactive waste was investigated. The first aim of the research was to evaluate the influence of the process parameters on the treatment of model solutions with different compositions. Subsequent experimental tests were conducted using solutions containing selected radionuclides (60Co and 137Cs), which are potential contaminants of effluents from nuclear power plants, as well as components often found in waste generated from industrial and medical radioisotope applications. The results of the experiments performed on real radioactive waste confirmed that electrodialysis was a suitable method for the treatment of such effluents because it ensured high levels of desalination and rates of decontamination. The most important parameters impacting the process were the applied voltage and electrical current. Moreover, this research shows that the application of the ED process enables the separation of non-ionic organic contaminants of LLW, which are unfavorable in further stages of waste predisposal.

Sewage sludge ash contaminated with radiocesium: Solidification with alkaline-reacted metakaolinite (geopolymer) and Portland cement

This study contributes toward developing measures for the disposal of radiocesium-contaminated sewage sludge ash (SSA). Here, we prepared two types of solidified bodies containing 30 wt% radiocesium-bearing SSA. The material used for the two solidified bodies were alkaline-reacted metakaolinite (geopolymer) and ordinary Portland cement (OPC). Cement has been used for solidification of low-level radioactive wastes, and geopolymer is a candidate of cement alternative materials. The characteristics of these solidified bodies were investigated by various aspects including mechanical strength, transformation of SSA components during solidification, and radiocesium confinement ability by leaching test. The compressive strength of geopolymer- and OPC-solidified bodies at 30 wt% SSA content was more than 40 MPa. After static leaching test at 60 °C, 137Cs was hardly leached out from the geopolymer-solidified bodies containing SSA at 30 wt% to ultrapure water (<0.1%), whereas more than 30% 137Cs was leached from the OPC-solidified bodies containing SSA at 30 wt% even though only ~9% of 137Cs in the SSA is soluble. These results strongly indicate that geopolymer is far superior to OPC for solidifying radiocesium-bearing SSA.

Adsorption of U(VI) on the natural soil around a very low-level waste repository

The behaviors of U(VI) in environmental media around radioactive waste disposal site are important for safety assessment of geological repositories. However, the estimation of environmental behaviors of U(VI) in natural media was insufficient. This work aimed to determine the adsorption of U(VI) on natural soil surrounding a candidate very low-level radioactive waste (VLLW) disposal site in southwest China. Results showed that the adsorption process of U(VI) on soils could be well supported by pseudo-second-order kinetic and Freundlich model. The adsorption of U(VI) was pH-dependent but temperature-independent. High ionic strength (NaCl) strongly affected the adsorption process at low pH (2.0–5.5). CO32− remarkably inhibited the U(VI) adsorption, while the adsorption of U(VI) was promoted by PO43− and SO42−. Naturally occurred soil organic matters (SOMs) showed high affinity for U(VI), while the presence of additional humic acid (HA) strongly inhibited U(VI) adsorption. The occurrence of ferrous iron could result in the reduction of U(VI) at low pH values (pH < 4), leading to the promotion of immobilization of U(VI). These findings would provide some guidance for the safety assessments of the VLLW disposal as well as the remediation of contaminated soil.

Status of Czech Low and Intermediate Radioactive Waste Management in the Context of European Development

The article summarises the status and competence of UJV Rez, a. s. (up to 2012, the Nuclear Research Institute Rez, Czech Republic) in the field of radioactive waste (RAW) management as a company managing of 95% of institutional radioactive wastes in Czech Republic. UJV Rez a. s. has been one of the Czech Republic’s key research and engineering institutions in the field of nuclear energy production since 1955. The company processes and conditions prior to storage 95% of so-called institutional RAW and is the principal partner of the state with respect to the research support of the Czech deep geological repository development project. UJV Rez a. s. boasts its own accredited radiochemical analytical test laboratory, unique of its kind in the Czech Republic. Of equal importance is UJV Rez’s active participation in a range of international organisations and associations and its involvement in wide range of international projects, and so as European projects. One of them is EU funded project PREDIS: Pre-disposal management of radioactive wastes, that has started at September 2020, focused on the field of low level radioactive waste (LLW) and intermediate level radioactive waste (ILW) pre-disposal.

Preparation of the Applicable Regulatory Guideline on Mixed Waste in Korea Based on the Analysis of US Laws and Regulations

Unit 1 of the Kori Nuclear Power Plant (NPP) and Unit 1 of the Wolsong NPP are being prepared for decommissioning; their decommissioning is expected to generate large amounts of intermediate-level, low-level, and very low level Waste. Mixed waste containing both radioactive and hazardous substances is expected to be produced. Nevertheless, laws and regulations, such as the Korean Nuclear Safety Act and Waste Management Act, do not define clear regulatory guidelines for mixed waste. However, the United States has strictly enforced regulations on mixed waste, focusing on the human health and environmental effects of its hazardous components. The U.S. Nuclear Regulatory Commission and the U.S. Department of Energy regulate the radioactive components of mixed waste under the Atomic Energy Act. The U.S. Environmental Protection Agency regulates the hazardous waste component of mixed waste under the Resource Conservation and Recovery Act. In this study, the laws, regulations, and authorities pertaining to mixed waste in the United States are reviewed. Through comparison and analysis with waste management laws and regulations in Korea, a treatment direction for mixed waste is suggested. Such a treatment for mixed waste will increase the efficiency of managing mixed waste when decommissioning NPPs in the near future.

A Study About Radionuclides Migration Behavior in Terms of Solubility at Gyeongju Low- and Intermediate-Level Radioactive Waste (LILW) Repository

A safety assessment of radioactive waste repositories is a mandatory requirement process because there are possible radiological hazards owing to radionuclide migration from radioactive waste to the biosphere. For a reliable safety assessment, it is important to establish a parameter database that reflects the site-specific characteristics of the disposal facility and repository site. From this perspective, solubility, a major geochemical parameter, has been chosen as an important parameter for modeling the migration behavior of radionuclides. The solubilities were derived for Am, Ni, Tc, and U, which were major radionuclides in this study, and on-site groundwater data reflecting the operational conditions of the Gyeongju low and intermediate level radioactive waste (LILW) repository were applied to reflect the site-specific characteristics. The radiation dose was derived by applying the solubility and radionuclide inventory data to the RESRAD-OFFSITE code, and sensitivity analysis of the dose according to the solubility variation was performed. As a result, owing to the low amount of radionuclide inventory, the dose variation was insignificant. The derived solubility can be used as the main input data for the safety assessment of the Gyeongju LILW repository in the future.

Bio-Dissolution Process as Environmental Technology for Uranium Leaching from El-Sella Ore Material by Aspergillus sulphureus

Research into radionuclide leaching behavior in the treatment of low-level radioactive waste solidification has been a widespread concern. Bioleaching of uranium was carried out using Aspergillus sulphureus isolated from El-Sella ore material. This area is located in the southern eastern desert of Egypt. The maximum bioleaching of U(VI) was found to be 83.1 % at these optimum conditions: 9 days incubation period, 0.5% pulp density, 30 °C incubation temperature at shaking speed 175 rpm. Glucose and NH4Cl were considered the best carbon and nitrogen sources for fungal growth through direct bioleaching process. A. sulphureus exhibits good potential in generating varieties of organic acids which effective for bioleaching of uranium. It produced 45.2 and 17 µg/ml from gallic and ellagic acids, respectively in the culture filtrate under the optimum conditions. This work represented the environmental technology for leaching of uranium where this is method is more save and low cost.

Environmental impact of amino acids on the release of selenate immobilized in hydrotalcite: Integrated interpretation of experimental and density-functional theory study

The environmental impact of amino acids on the release of SeO42− immobilized into hydrotalcite (Mg2Al-LDH) which belongs to the layered double hydroxides (LDHs) family was investigated by experimental study and the observed layer structure of hydrotalcite was verified through density-functional theory (DFT) calculations. Glycine, l-cysteine, and l-aspartic acid, which have smaller molecular sizes, can release SeO42− largely due to intercalation, unstabilization of Mg2Al-LDH and simple dissolution, while l-tryptophan and l-phenylalanine caused limited SeO42− release due to their larger sizes and aromaticity. XRD patterns for the solid residues after intercalation of amino acids revealed that the layer distance of Mg2Al-LDH was partially expanded. The main peaks and shoulder features corresponding to d003 diffraction were well explained by DFT simulations using glycine as a model: the layer spacing of the main peak is responsible for the remaining SeO42− and singly stacked glycine molecule and the layer spacing of the shoulder peak was well explained by doubly stacked glycine molecules. Hydrogen bonds between amino acids and hydroxyl ions in the metallic layers of Mg2Al-LDH were responsible for the stable configuration of the intercalated Mg2Al-LDH. This study indicates potential limitations to the stability of low-level radioactive wastes of 79Se in repositories which are affected by smaller molecules of amino acids released through degradation of organic matters in the pedosphere.

Technical Management Assessment Guide to Historically Solid Radioactive Materials (Classes LLW and ILW): Case Study of the Greek Nuclear Research Reactor (GRR-1)

Abstract The purpose of this work is the radioactive control of long-term-stored materials [historically radioactive waste, Types LLW (low-level waste) and ILW (intermediate-level waste)] in an int...

Waste expectations of fusion steels under current waste repository criteria

During operation fusion reactor components will be exposed to long periods of neutron irradiation. As such, a reactor’s structural steels will become activated and need to be disposed of as radioactive waste. Previous studies have shown that such wastes can struggle to meet low level waste (LLW) requirements meaning that costly geological disposal may be required. In order to explore the waste expectations of steels from European DEMO-like fusion reactors, several radioactive waste management systems have been investigated. This includes their LLW criteria, currently available disposal sites and planned future developments. This information was used to analyse the results of DEMO-like inventory simulations of potential reactor steels. The simulations were performed with the inventory code FISPACT-II and the TENDL2017 nuclear data library. The results suggest that when steels are exposed to near plasma neutron fluxes they will struggle to meet the majority of LLW requirements. For lower neutron fluxes, typical of reactor containment vessels, the waste expectations can be more positive, with several steels able to meet some low level criteria. It can be concluded that steels should not be expected to be consistently internationally classified as LLW 100 years after reactor shut down. As all activated fusion waste cannot be disposed of in a single location, it is recommended that waste disposal strategies are included in any fusion reactor proposal before construction begins. These strategies need to align with the radioactive waste regulations the proposed reactor will be subject to.

Dynamic cost analysis for disposal of low and intermediate level nuclear waste in China

The management and financial problems of nuclear waste have raised the concern worldwide due to lack of experience in decommissioning and disposal. In this paper, a primary cost estimation model is proposed based on Activity-based Life Cycle Costing (AB-LCC) approach in order to influence the strategy of Low and Intermediate Level Waste (LILW) disposal in China. AB-LCC model provides a dynamic cost estimation of LILW disposal and its application is not restricted by the region and time. A dynamic analysis of resources due to time and regional differences of LILW management during its life cycle time has been performed on the basis of Activity-based Costing (ABC) matrix. The static and dynamic costs of the primary and secondary activities at each stage of the disposal repositories are obtained. The model is verified by comparison with statistics from the cases of Aube repositories and difference is approximately less than 5%. Therefore AB-LCC model is used to estimate the LILW disposal costs in China with different disposal modes. Finally, LILW management strategy was suggested to the Chinese policy-makers that the Northwest Centralized Disposal Mode (NCDM) is more cost-saving than the Coastal Independent Disposal Mode (CIDM) and Gansu province is the most recommended disposal site for economic considerations.

COMPARISON OF WASTE DUE TO IRRADIATED STEELS IN THE ESFR AND DEMO

For either nuclear fusion or generation IV fission reactors to be viable as a commercial energy source the decommissioning and waste disposal solutions must be considered during the design. A multi-step simulation process combining Monte Carlo Neutron Transport simulations with inventory simulations have been performed to estimate the activation of steels in key reactor components of the European Sodium-cooled fast Reactor (ESFR). Waste classifications based on UK waste disposal regulations have been applied to the key components to estimate the expected masses of low level and intermediate level waste. The use of reduced activation steels, EUROFER and F82H, in reactor components external to the core results in a factor of 10 reduction in the percentage of waste classified as Intermediate Level Waste (ILW). Waste estimates are compared to existing waste estimates for the European Demonstration fusion reactor (DEMO). The ESFR has a lower percentage of ILW per total reactor mass due to irradiated steels compared to DEMO. However, there is no Higher Activity Waste (HAW) associated with DEMO, compared with arisings from the ESFR spent fission fuel.

Application of biosorbents in hybrid ultrafiltration/sorption processes to remove radionuclides from low-level radioactive waste

Application of biosorbents in hybrid ultrafiltration/sorption processes to remove radionuclides from low-level radioactive waste

WASTE CLASSIFICATION ASSESSMENT OF NUCLEAR STEELS FOR FUSION POWER APPLICATIONS

Fusion power is an attractive option for the world’s future energy needs. An important goal for fusion is to avoid the severe radioactive waste issues associated with nuclear fission. However, the neutrons produced in the fusion plasma reaction impinge on the surrounding reactor structure causing nuclear activation. It is hoped that activated material from fusion facilities can be disposed of as low level waste 50-100 years after operation ceases, but recent work suggests this may be difficult to achieve. This work presents inventory simulations for a number of potential fusion steels, for two neutron irradiation conditions typical of the DEMO reactor concept. The results are used to determine if the steels meet low level waste regulations, for a number of different international waste management systems. These results show that steels do not appear able to consistently meet low level waste requirements when exposed to near-plasma neutron fluxes. They have more success when exposed to lower fluxes, but traditional steels will still struggle to meet low level waste requirements in a fusion environment.