The operation of nuclear facilities involves the potential for on-site contamination of soil, primarily resulting from pipe leaks and other operational incidents. Globally, decommissioning process for commercial nuclear power plants have revealed huge-amounts of soil waste contaminated with Cs-137, Sr-90, Co-60, and H-3. For example, Connecticut Yankee in the United States produced approximately 52,800 ton of contaminated soil waste, constituting 10% of the total waste generated during its decommissioning. Environmental remediation costs associated with nuclear decommissioning in the US averaged $60 million per unit, representing a significant 10% of the whole decommissioning expenses. Consequently, this study undertook a preliminary investigation to identify important factors for establishing a site remediation strategy based on radionuclide- and site-specific media- characteristics, focusing the efficiency enhancement for the environmental remediation. The factors considered for this investigation were categorized into physical/environmental, socioeconomic, technical, and management aspects. Physical/environmental factors contained the site characteristics, contamination levels, and environmental sensitivity, while socio-economic factors included the social concerns and economic costs. Technical and management factors included subcategories such as technical considerations, policy aspects, and management factors. Especially, technical factors were further subdivided to consider the site reuse potential, secondary waste generation by site remediation, remediation efficiency, and remediation time. Additionally, our study focused the key factors that facilitate the systematic planning for the site remediation, considering the distribution coefficient (Kd) and hydrogeological characteristics associated with each radionuclide in specific site conditions. Therefore, key factors in this study focus the geochemical characteristics of site media including the particle size distribution, chemical composition, organic and inorganic constituents, and soil moisture content. Moreover, the adsorption properties of site media were examined concerning the distribution coefficient (Kd) of radionuclides and their migration characteristics. Furthermore, this study supported the development of a conceptual framework, containing the remediation strategies that incorporate the mobility of radionuclides, according to the site-specific media. This conceptual framework would necessitate the spatial analysis techniques involving the whole contamination surveys and radionuclide mobility modeling data. By integrating these key factors, the study provides the selection and simulation of optimal remediation methods, ultimately offering the estimated amounts of radioactive waste and its disposal costs. Therefore, these key factors offer foundational insights for designing the site remediation strategies according the sitespecific information such as the distribution coefficient (Kd) and hydrogeological characteristics.
The physicochemical similarities of hydrogen isotopes have made their separation a challenging task. Conventional methods such as cryogenic distillation, Girdler sulfide process, chromatography, and thermal cycling absorption have low separation factors and are energy-intensive. To overcome these limitations, research has focused on kinetic quantum sieving (KQS) and chemical affinity quantum sieving (CAQS) effects for selective separation of hydrogen isotopes. Porous materials such as metal-organic frameworks (MOF), covalent organic frameworks (COF), zeolites, carbon, and organic cages have been studied for hydrogen separation. In this study, we focus the enhancement for CAQS to provide the cations due to the chemical affinity between hydrogen isotope and unsaturated sites by cations in zeolite beads. Cation exchanged zeolite beads was synthesized with cobalt, copper, nickel, iron and silver in zeolite 4A beads. Synthesized cation exchanged zeolite was analyzed for the surface area and pore size in N2 and adsorption behaviors of hydrogen isotopes (D2/H2) for various cation exchanged zeolite beads using BET at 77 K. The study predicts the D2/H2 adsorption selectivity based on the results obtained with BET. These hydrogen isotope adsorption results will provide a foundation for future processes for tritium separation.
General phases in the plan and implementation of an environmental remediation of radioactively contaminated sites are planning for remediation, site characterization, remediation criteria, remediation strategy, implementing remediation actions, and conducting post-remediation activities. Environmental remediation should commence with a planning stage. It is helpful to prepare reports which detail all the supporting activities related to these elements before significant levels of funds and efforts are committed. Site characterization is needed to provide sufficient data to make strategic decisions on the environmental remediation activities. The source characterization should include both waste characterization and facility or site characterization and should provide reliable estimates of the release rates of radioactive constituents as well as constituent distribution. During the preliminary site characterization, an engineering study should be conducted to develop remediation options which address the specific contaminant problem and are aimed to reduce radiological and chemical exposure. Options will include engineering approaches and associated technologies. A preliminary selection of options may be made based on several factors including future sites use, technical considerations, public acceptability, cost, and regulatory requirements. The implementation of remediation actions includes procurement of the selected technology, preparation of the site, development of a health and safety plan, development of operations procedures, staff selection and training, completion of site cleanup, verification, waste disposal, and release of the site for any future use. Once remediation activities have been completed and verified, the remediated site can be released for restricted or unrestricted use. Remediation of radioactively contaminated sites may require special adaptation to address sites covering very large surface areas or those which are deep and difficult to access. Quality assurance may be very important to the verification of environmental remediation activities. The selection of optimal remediation technologies to solve or mitigate the safety of an environmental contamination problem should be taken into account several factors. The several factors include performance (the ability of the technology to reduce risk to the health and safety of the public and to the environment), reliability and maintenance requirements for the technology, costs of implementing the technology, infrastructure available to support the technology, availability(the ease of accessing the technology and associated services), risk to workers and public safety, environmental impacts of the technology, ability of the technology to meet regulatory acceptance, and communication of stakeholder.
Nuclear facilities present the important task related to the migration and retention of radioactive contaminants such as cesium (Cs), strontium (Sr), and cobalt (Co) for unexpected events in various environmental conditions. The distribution coefficient (Kd) is important factor for understanding these contaminants mobility, influenced by environmental variables. This study focusses the prediction of Kd values for radionuclides within solid phase groups through the application of machine-learning models trained on experimental data and open source data from Japan atomic energy agency. Three machine-learning models, such as the convolutional neural network, artificial neural network, and random forest, were trained for prediction model of the distribution coefficient (Kd). Fourteen input variables drawn from the database and experimental data, including parameters such as initial concentration, solid-phase characteristics, and solution conditions, served as the basis for model training. To enhance model performance, these variables underwent preprocessing steps involving normalization and log transformation. The performances of the models were evaluated using the coefficient of determination. These results showed that the environmental media, initial radionuclide concentration, solid phase properties, and solution conditions were significant variables for Kd prediction. These models accurately predict Kd values for different environmental conditions and can assess the environmental risk by analyzing the behavior of radionuclides in solid phase groups. The results of this study can improve safety analyses and longterm risk assessments related to waste disposal and prevent potential hazards and sources of contamination in the surrounding environment.
The separation of hydrogen isotopes is a critical issue in various fields, such as deuterium or tritium production and the treatment of radioactively contaminated water. In this presentation, we describe the pervaporative separation of hydrogen isotopes using proton conductive membranes and underlying separation mechanism. We investigated the H/D separation factors of perfluorosulfonic acid (Nafion) and polybenzimidazole membranes using pervaporation, and found that both membranes exhibited similar separation factors of approximately 1.026. Water permeation flux through the membranes was highly dependent on their thickness and type, and increased with operation temperature. However, the effect of temperature on H/D separation factor was negligible. We also demonstrated the cascade separation of H/D, indicating the potential application of multi-stage operation. We found that surface transport mechanisms such as hydron hopping contributed the most to H/D separation during the pervaporation process of proton conductive membranes.
The physicochemical similarities of hydrogen isotopes have made their separation a challenging task. Conventional methods such as cryogenic distillation, Girdler sulfide process, chromatography, and thermal cycling absorption have low separation factors and are energy-intensive. To overcome these limitations, research has focused on kinetic quantum sieving (KQS) and chemical affinity quantum sieving (CAQS) effects for selective separation of hydrogen isotopes. Porous materials such as metal-organic frameworks (MOF), covalent organic frameworks (COF), zeolites, carbon, and organic cages have been studied for hydrogen separation. This study have the literature review for previous research on D2/H2 adsorption and analyzes the D2/H2 adsorption behaviors of hydrogen isotopes for various zeolite using BET at 77 K. The study predicts the D2/H2 adsorption selectivity based on the results obtained with BET. These hydrogen isotope adsorption fundamentals provide a foundation for future processes for tritium separation.
The mobility of radionuclides is largely determined by their radiological properties, geochemical conditions, and adsorption reactions, such as surface adsorption, chemical precipitation, and ion exchange. To evaluate the safety assessments of radionuclides in nuclear sites, it is essential to understand the behavior and mechanism of radionuclides onto soils. Since nuclear power plants are located in coastal areas, the chemical composition of groundwater can vary depending on the intrusion of seawater, altering the adsorption distribution coefficient (Kd) values of radionuclides. This study examines the impact of seawater on the Kd values of clay minerals for cesium (Cs) and strontium (Sr). The results of Cs+ adsorption experiments showed a broad range of Kd values from 36 to 1,820 mL/g at an initial concentration of 1 mg/L and a high sorption coefficient of 15-613 mL/g at an initial concentration of 10 mg/L. Montmorillonite, hydrobiotite, illite, and kaolinite were ranked in terms of their CEC values for Cs+ adsorption, with hydrobiotite having the highest adsorption at 1 mg/L. The results of Sr adsorption experiments showed a wide range of Kd values from 82 to 1,209 mL/g at an initial concentration of 1 mg/L and a lower adsorption coefficient of 6.68-344 mL/g at an initial concentration of 10 mg/L. Both Cs+ and Sr2+ demonstrated lower Kd values at higher initial concentrations. CEC of clays found to have a significant impact on Sr2+ Kd values. Ca2+ ions showed a significant impact on Sr2+ adsorption distribution coefficients, demonstrating the greater impact of seawater on Sr2+ compared to Cs+. These findings can inform future safety assessments of radionuclides in nuclear sites.
Radioactive contaminants, such as 137Cs, are a significant concern for long-term storage of nuclear waste. Migration and retention of these contaminants in various environmental media can pose a risk to the surrounding environment. The distribution coefficient (Kd) is a critical parameter for assessing the behavior of these contaminants and can introduce significant errors in predicting migration and remediation options. Accurate prediction of Kd values is essential to assess the behavior of radioactive contaminants and to ensure environmental safety. In this study, we present machine learning models based on the Japan Atomic Energy Agency Sorption Database (JAEA-SDB) to predict Kd values for Cs in soils. We used three different machine learning models, namely the random forest (RF), artificial neural network (ANN), and convolutional neural network (CNN), to predict Kd values. The models were trained on 14 input variables from the JAEA-SDB, including factors such as Cs concentration, solid phase properties, and solution conditions which are preprocessed by normalization and log transformation. We evaluated the performance of our models using the coefficient of determination (R2) value. The RF, ANN, and CNN models achieved R2 values of over 0.97, 0.86, and 0.88, respectively. Additionally, we analyzed the variable importance of RF using out-of-bag (OOB) and CNN with an attention module. Our results showed that the initial radionuclide concentration and properties of solid phase were important variables for Kd prediction. Our machine learning models provide accurate predictions of Kd values for different soil conditions. The Kd values predicted by our models can be used to assess the behavior of radioactive contaminants in various environmental media. This can help in predicting the potential migration and retention of contaminants in soils and the selection of appropriate site remediation options. Our study provides a reliable and efficient method for predicting Kd values that can be used in environmental risk assessment and waste management.
Working during decommissioning of nuclear facilities can subject workers to a number of industrial health and safety risks. Such facilities can contain hazardous processes and materials such as hot steam, harsh chemicals, electricity, pressurized fluids and mechanical hazards. Workers can be exposed to these and other hazards during normal duties (including slips, trips and falls, driving accidents and drowning). Industrial safety accidents, along with their direct impacts on the individuals involved, can negatively affect the image of nuclear facilities and their general acceptance by the public. Industrial safety is the condition of being protected from physical danger as a result of workplace conditions. Industrial safety program in a nuclear context are the policies and protections put in place to ensure nuclear facility workers are protected from hazards that could cause injury or illness. Preventive actions are those that detect, preclude or mitigate the degradation of a situation. They can be conducted regularly or periodically, one time in a planned manner, or in a predictive manner based on an observed condition. Corrective actions are those that restore a failed or degraded condition to its desired state based on observation of the failure or degradation. In industrial safety, the situations or conditions of interest are those observed via the performance monitoring, investigations, audits and management reviews. Preventive and corrective actions are those designed to place or return the system to its desired state. Preventive actions where possible are preferred as they eliminate the adverse condition prior to it occurring. When an accident or incident occurs, the primary focus is on obtaining appropriate treatment for injured people and securing the scene to prevent additional hazards or injuries. Once the injured personnel have been cared for and the scene has been secured, it is necessary to initiate a formal investigation to determine the extent of the damage, causal factors and corrective actions to be implemented. Certain tools may be needed to investigate such incidents and accidents. Initial identification of evidence immediately following the incident includes a list of people, equipment and materials involved and a recording of environmental factors such as weather, illumination, temperature, noise, ventilation and physical factors such as fatigue and age of the workers. The five Ws (what, who, when, where and why) are useful to remember in investigation of incidents and accidents.
Despite of careful planning of decommissioning projects, there are often surprises when facilities are opened for dismantling purposes, or when material is removed from hot cells, etc. Unexpected incidents and findings during the decommissioning of nuclear facilities have been referred to in the past as unknowns. However, many of the problems encountered during implementation of decommissioning are well known, it is simply that they were not expected to arise. In some other cases, the problem may not have been encountered in the decommissioning team’s experience, forcing the development of new techniques, tools and procedures to address the unexpected problem, with the attendant delays and cost overruns that this often involves. Unknowns in decommissioning cannot be eliminated, regardless of the efforts applied. This is especially the case in old facilities where documentation may have been lost or where modifications were carried out without updates to reports. As a result, when planning for decommissioning, it is prudent to assume that such problems will occur, and ensure that arrangements are in place to deal with them when they arise. This approach will not only improve the efficiency of the decommissioning project, but will also improve the safety of the operations. One of the most common root causes of unexpected events in decommissioning is the lack of detailed design information or missing records of modifications, maintenance issues and incidents during operation. It is therefore necessary to check the completeness of design information in existing plants and to ensure that configuration management techniques are applied at all stages of the lifetime of a plant. In the case of a new plant, archiving samples of materials can be a valuable source of information to support decommissioning planning. During the lifetime of plants, it is likely that modifications will be carried out involving the construction of new buildings. The opportunity should be taken in these circumstances to consider the layout, the physical size and other attributes of the plant to ensure that they do not make decommissioning of existing facilities more difficult and also to optimize the potential for reuse in support of the decommissioning of the whole site, later in the life of the facility. Characterization of all aspects of a plant is essential to reduce the number of unknowns and the likelihood of unexpected events. This characterization should be extensive, but there is a limit to the level of detail that should be sought as the cost versus benefit gain may reduce. Reducing unknowns by retrospectively obtaining physical data associated with a facility is a useful means of characterization, and there are many tools in existence that can be used to carry this out accurately and effectively. Regardless of the efforts that are employed in decommissioning planning, unexpected events should be anticipated and contingency plans prepared. Although the details of the event itself may not be anticipated, its impact may affect safety and environmental discharge, and may or may not involve radiological impacts. Regardless of more serious impacts, unexpected events are likely to result in modifications to the decommissioning plan, incur delays and cost money. Finally, regardless of the status of a facility, whether at the concept stage or at the decommissioning stage of its life cycle, it is never too early to begin thinking and planning for decommissioning.
The removal of cesium (Cs) from contaminated clay minerals is still a challenge due to the limited efficiency of the process. Thus, this study aimed to enhance the removal for Cs+ ions during the conventional acid washing process by incorporating a bead-type adsorbent. Polyacrylonitrile-based nickel potassium hexacyanoferrate (NiFC-PAN) was utilized as the Cs adsorbent to selectively adsorb Cs+ ions in a strongly acidic solution that contained competing ions. To enable easy separation of clay particles and protect the adsorbent from harsh environmental conditions, PAN was deliberately constructed as large beads. The synthesized adsorbent (NiFC/PAN in a 2:1 ratio) displayed high selectivity for Cs+ ions and had a maximum capacity of 162.78 mg/g for Cs+ adsorption in 0.5 M HNO3 solution. Since NiFC-PAN exhibited greater Cs selectivity than the clay mineral (hydrobiotite, HBT), adding NiFC-PAN during the acid washing substantially increased Cs desorption (73.3%) by preventing the re-adsorption for Cs+ ions on the HBT. The acid treatment in the presence of NiFCPAN also significantly decreased the radioactivity of 137Cs-HBT from 209 to 27 Bq/g, resulting in a desorption efficiency of 87.1%. Therefore, these findings suggest that the proposed technique is a potentially useful and effective method for decontaminating radioactive clay.
Hydrogen isotopes (H, D, T) separation technologies have received great interest for treatments of tritiated liquid waste produced in Fukushima. In addition, the separated deuterium and tritium can be utilized in various industries such as semiconductors and nuclear fusion as expensive and rare resources. However, separating hydrogen isotopes in gas and liquid forms still requires energyintensive processes. To improve efficiency and performance of hydrogen isotope separation, we are developing water electrolysis, cryosorption, distillation, isotope exchange, and hydrophobic catalyst technologies. Furthermore, an analytical method is studied to evaluate the separation of hydrogen isotopes. This presentation introduces the current status of hydrogen isotope research in this research group.
A large spectrum of possible stakeholders and important factors for safety improvement during decommissioning of nuclear facilities should be identified. Decommissioning includes additional aspects which are of interest to a wider range of stakeholders. The way in which local communities, the public in general, and a wide range of other parties are engaged in dialogue about decommissioning of nuclear facilities is likely to become an increasingly important issue as the scale of the activity grows. Timely stakeholder involvement may enhance safety and can encourage public confidence. Stakeholder engagement may result in attention to issues that otherwise might escape scrutiny. Public confidence is improved if issues that are raised by the public are taken seriously and are carefully and openly evaluated. Experience in many countries has shown that transparency can be an extremely effective tool to enhance safety performance. It sets out the development and implementation of an effective two-way process between the organization and stakeholders. Meaningful engagement is characterized through a flow of communication, opinions and proposals in both directions and the use of collaborative approaches to influence and explain decisions. The process is one in which an organization learns and improves its ability to perform meaningful stakeholder engagement while developing relationships of mutual respect, in place of one-off consultations. The evolving nature of this process is particularly relevant to pipeline projects, which will have differing stakeholder engagement requirements at each phase of the project lifecycle. Activity undertaken at all stages of the process should be documented to ensure engagement success can be reviewed and improved and to ensure historical decisions or engagements are captured in case stakeholders change during the progression of time and previous consultation records are required.
An induction melting facility includes several work health and safety risks. To manage the work health and safety risks, care must be taken to identify reasonably foreseeable hazards that could give rise to risks to health and safety, to eliminate risks to health and safety so far as is reasonably practicable. If it is not reasonably practicable to eliminate risks to health and safety, attention have to be given to minimize those risks so far as is reasonably practicable by implementing risk control measures according to the hierarchy of control in regulation, to ensure the control measure is, and is maintained so that it remains, effective, and to review and as necessary revise control measures implemented to maintain, so far as is reasonably practicable, a work environment that is without risks to health or safety. The way to manage the risks associated with induction melting works is to identify hazards and find out what could cause harm from melting works, to assess risks if necessary – understand the nature of the harm that could be caused by the hazard, how serious the harm could be and the likelihood of it happening, to control risks – implement the most effective control measures that are reasonably practicable in the circumstances, and to review control measures to ensure they are working as planned.
Water electrolysis is a representative technology for tritium enrichment in water. Proton exchange membrane (PEM) water electrolysis has received great attention to replace traditional alkaline water electrolysis which generates concentrated tritiated water containing a large amount of salts. Nafion has been widely used as a polymeric electrolyte for the PEM electrolyzer. However, its low gas barrier property causes explosion, corrosion or degradation of electrolyzer. Furthermore, the traditional polymeric electrolytes have negligible differences in conductivity between hydrogen isotopes. To enhance the tritium separation by water electrolysis, we designed a composite membrane (Nafion/ hexagonal boron nitride (hBN)). The monolayer hBN has a high proton conductivity and gas barrier property, and the hBN can enhance conductivity differences between hydrogen isotopes. We prepared Nafion/hBN composite membranes, and water electrolysis performances and proton/deuterium separation behaviors were investigated.
Detritiation of low-level tritiated water has become global issue after Fukushima accident. Several attempts have been made to reduce the radioactivity of Fukushima tritiated water below legal limit of nuclear plant effluents (~104 Bq·L−1). Various technologies such as water distillation, electrolysis, and catalytic exchange were tested to treat the tritiated water, however, those demand enormous expense to achieve the goal due to low process efficiency. It highlights that the performance enhancement of current technologies is necessary to improve economic feasibility. We have quantitatively evaluated the separation performance of various polymers toward low-level tritium (~105 Bq·L−1) through batch experiments. The polystyrene with grafted by 20 types of functional groups (Tris (2-aminoethyl) amine, dimethylaminomethyl, isocyanate, mercaptomethyl, aminomethyl, hydroxymethyl, triphenylphosphine, morpholine, 2-chlorotrityl amine, 4-(dimethylamino) pyridine, poly (vinyl chloride) carboxylated, poly (4-vinyl pyridine), p-toluenesulfonic acid, p-toluenesulfonyl hydrazide, piperidine, acetyl polystyrene, 2-chlorotrityl chloride, piperazine, diethylene triamine, poly (vinyl chloride)) were suspended in HTO solution (initial activity = 4.7 × 105 Bq·L−1). After the equilibration, the suspension was filtered using 3 kDa membrane filter and the activity in filtrates were quantified by LSC (HIDEX-300 SL). The results demonstrate the detritiation efficiency and separation factors of functional groups toward tritium. Carboxylic group (COOH) showed the most reactive performance as detritiation efficiency of ~4%. Compared to other functional groups, styrene sulfonyl groups including sulfonyl amide (SNH2) and sulfonyl hydrazide (SNHNH2) revealed promising performance for tritium separation as separation factor of 10.97 and 3.85, respectively. However, sulfonyl hydroxide (SOH) which is known as reactive functional group to tritium exchange showed the poor performance (detritiation efficiency: 0.68%; separation factor: 3.02). This study could suggest the promising functional groups for detritiation of low-level tritiated water which can be utilized to enhance the performance of current technologies. For example, reactive functional groups can be grafted on the surface of packing material within distillation tower resulting in the increasing detritiation efficiency.
A large amount of acidic wastewater was generated from the soil washing process. This study focuses on the capture for the radionuclide, especially cesium (Cs), in soil washing wastewater. We conducted the two-step process to reduce the amount of radioactive wastewater after soil washing using the coagulants and adsorbents in each step. We synthesized the adsorbent to capture Cs radionuclides in acidic wastewater (pH < 1). Based on the results, we found that the optimum ratio (NiFC:PAN) was 3.5:1 for the removal efficiency and strength of adsorbent. We compare the NiFC powder and NiFC-PAN for removal efficiency and separation of adsorbent after batch test, showing that the removal efficiency and separation of NiFC-PAN was lower and higher than NiFC power, respectively. We conducted the radioactive experiment to evaluate the satisfaction below release criteria (< 10 Bq·L−1, Cs), reporting that NIFC-PAN adsorbent meet the release criteria. These results showed that NiFC-PAN is promising adsorbent for Cs capture in strong acidic wastewater generated from soil washing and separation after capture process.