Current Status of the Radioactive Waste Management Programme in Spain

Since 1984, ENRESA is responsible of the radioactive waste management and the decommissioning of nuclear installations in Spain. The major recent challenge has been the approval of the Sixth General Radioactive Waste Plan (GRWP) as “master plan” of the activities to be performed by ENRESA. Regarding the LILW programme, the El Cabril LILW disposal facility will be described highlighting the most relevant events especially focused on optimizing the existing capacity and the start-up of a purpose–built disposal area for VLLW. Concerning the HLW programme, two aspects may be distinguished in the direct management of spent fuel: temporary storage and long-term management. In this regards, a major challenge has been the decision adopted by the Spanish Government to set up a Interministerial Committee for the establishment of the criteria that must be met by the site of the Centralized Intermediate Storage (CTS) facility as the first and necessary step for the process. Also the developments of the long-term management programme will be presented in the frame of the ENRESA’s R&D programme. Finally, in the field of decommissioning they will be presented the PIMIC project at the CIEMAT centre and the activities in course for the decommissioning of Jose´ Cabrera NPP.

ISO Standardization of the Scaling Factor Method for Low- and Intermediate Level Radioactive Wastes Generated at Nuclear Power Plants

Low- and intermediate-level radioactive wastes (L-ILW) generated at nuclear power plants are disposed of in various countries. In the disposal of such wastes, it is required that the radioactivity concentrations of waste packages should be declared with respect to difficult-to-measure nuclides (DTM nuclides), such as C-14, Ni-63 and α-emitting nuclides, which are often limited to maximum values in disposal licenses, safety cases and/or regulations for maximum radioactive concentrations. To fulfill this requirement, the Scaling Factor method (SF method) has been applied in various countries as a principal method for determining the concentrations of DTM nuclides. In the SF method, the concentrations of DTM nuclides are determined by multiplying the concentrations of certain key nuclides by SF values (the determined ratios of radioactive concentration between DTM nuclides and those key nuclides). The SF values used as conversion factors are determined from the correlation between DTM nuclides and key nuclides such as Co-60. The concentrations of key nuclides are determined by γ ray measurements which can be made comparatively easily from outside the waste package. The SF values are calculated based on the data obtained from the radiochemical analysis of waste samples. The use of SFs, which are empirically based on analytical data, has become established as a widely recognized “de facto standard”. A number of countries have independently collected nuclide data by analysis over many years and each has developed its own SF method, but all the SF methods that have been adopted are similar. The project team for standardization had been organized for establishing this SF method as a “de jure standard” in the international standardization system of the International Organization for Standardization (ISO). The project team for standardization has advanced the standardization through technical studies, based upon each country’s study results and analysis data. The conclusions reached by the project team was published as ISO International Standard 21238:2007 “The Scaling Factor method to determine the radioactivity of low- and intermediate-level radioactive waste packages generated at nuclear power plants” [1]. This paper gives an introduction to the international standardization process for the SF method and the contents of the recently published International Standard.

Characteristics of Solidified Products Containing Radioactive Molten Salt Waste

For a treatment of molten salt wastes generated from a pyroprocessing of oxide spent fuel, we had suggested a stable chemical route, named GRSS (Gel-Route Stabilization & Solidification), and a subsequent consolidation method. By using this method, a series of monolithic wasteforms with different conditions were fabricated, and then their physicochemical properties were investigated. A simulated salt containing 90wt% LiCl, 6.8wt% CsCl, and 3.2wt% SrCl2 was treated with a gel-forming material system, Si/Al/P = 0.4/0.4/0.2 and 0.35/0.35/0.3, and the gel-products were treated at 1100C° after mixing with borosilicate glass powder, where the salt loadings were about 16∼20wt%. The solidified products had a density of 2.3∼2.35g/cm3, a micro-hardness of 4.69∼4.72GPa, a glass transition temperature of 528∼537C°, and a thermal expansion coefficient of 1.65×10−7∼3.38×10−5/C°. Leaching results by the PCT-A method revealed leached rates, 10−3∼10−2g/m2day and 10−4∼10−3g/m2day for Cs and Sr, respectively. From the long-term ISO leaching test, the 900day-leached fraction of Cs and Sr predicted by a semi-empirical model were 0.89% and 0.39%. The leaching behaviors indicated that Cs would be immobilized into a Si-rich phase while Sr would be in a P-rich phase. The experimental results revealed that the GRSS method could be an alternative method for a solidification of radioactive molten salt wastes.

Cost and Waste Volume Reduction in HEPA Filter Trains by Effective Pre-Filtration

Data published elsewhere (Moore, et al., 1992; Bergman et al., 1997) suggests that the then costs of disposable type Glass Fibre HEPA filtration trains to the DOE was $55million per year (based on an average usage of HEPA panels of 11,748 pieces per year between 1987 and 1990), $50million of which was attributable to installation, testing, removal and disposal. The same authors suggest that by 1995 the number of HEPA panels being used had dropped to an estimated 4000 pieces per year due to the ending of the Cold War. The yearly cost to the DOE of 4000 units per year was estimated to be $29.5 million using the same parameters that previously suggested the $55 million figure. Within that cost estimate, $300 each was the value given to the filter and $4,450 was given to peripheral activity per filter. Clearly, if the $4,450 component could be reduced, tremendous saving could result, in addition to a significant reduction in the legacy burden of waste volumes. This same cost is applied to both the 11,748 and 4000 usage figures. The work up to now has focussed on the development of a low cost, long life (cleanable), direct replacement of the traditional filter train. This paper will review an alternative strategy, that of preventing the contaminating dust from reaching and blinding the HEPA filters, and thereby removing the need to replace them. What has become clear is that ‘low cost’ and ‘Metallic HEPA’ are not compatible terms. The original Bergman et al., 1997 work suggested that 1000 cfm (cubic feet per minute) (1690 m3/hr) stainless HEPAs could be commercially available for $5000 each after development (although the $70,000 development unit may be somewhat exaggerated – the authors own company have estimated development units able to be retrofitted into strengthened standard housings would be available for perhaps $30,000). The likely true cost of such an item produced industrially in significant numbers may be closer to $15,000 each. That being the case, the economics for replacing glass fibre HEPAs with the metallic, cleanable alternative are unjustifiable except on ethical grounds. By proposing the protection of the traditional Glass Fibre HEPA from its blinding contamination, a means is presented to reduce both their life costs and ultimate waste volumes. An examination of the case for self-cleaning HEPA protection also suggests that, even when the mechanical life limit of the HEPA train is reached, the degree of contamination could be reduced to such an extent that its means/classification of final disposal may be modified to further reduce cost. Pulsed jet filtration using metallic filter media is a practical and industrially proven means by which solids can be prevented from reaching the HEPA train and returned to the operator for disposal, whilst not interrupting the process flow through the system. Field experience and data to prove the contention is available. There are clearly benefits with regard to disposal in returning to the user the small quantities of dust that would otherwise lead to the contamination and blinding of the large volume of the filter train. A cost benefit analysis shows that this radical solution to HEPA cost amelioration can work. Presenting a review of the technology and its application to other areas illustrates that where gross dust removal or recovery is necessary, or where extreme conditions make traditional HEPA technologies impractical, metallic filtration systems can (and do) also offer economic and industrially real solutions.

The Crucial Importance of the Back-End in Multinational Initiatives to Enhance Fuel Cycle Security

There have been repeated proposals for establishing multinational cooperation approaches that could reduce the security concerns of spreading nuclear technologies. Most recently, there have been initiatives by both Russia (GNPI) and the USA (GNEP) – each aimed at promoting nuclear power whilst limiting security concerns. In practice, both initiatives place emphasis on the supply of reactors and enriched fuel but neither has made clear and specific proposals about the back-end part of the arrangement. The primary incentive offered to the user countries is “security of supply” of the front end services. However, there is no current shortage of supply of front end services, so that the incentives are not large. A much greater incentive could be the provision of a spent fuel or waste disposal service. The fuel supplied to Tier 2 countries could be shipped back (with no return of wastes) to the supplier or else to an accepted third party country that is trusted to operate safe and secure disposal facilities. If a comprehensive service that obviates the need for a national deep repository is offered to small countries then there will be a really strong incentive for them to sign up to GNEP or GNPI type deals.

Experimental Investigation on the Volume Reduction of Irradiated Graphite Arising From the Decommissioning of KRR-2

Graphite has been used as a moderator and reflector of neutrons in more than 100 nuclear power plants as well as many experimental reactors and plutonium production reactors in various countries. Most of the older graphite moderated reactors are already shut down and are awaiting decommissioning planning and preparation. The graphite waste has different characteristics than other decommissioning waste due to its physical and chemical properties and also because of the presence of tritium and carbon-14. Therefore radioactive graphite dismantling, handling, conditioning and disposal are a common part of the decommissioning activities. A volume reduction of the waste is needed to reduce disposal cost of radioactive waste. However the existing processing technologies are based mostly on the isolation of radioactive graphite from the environment, they are not able to provide for a significant volume reduction. For this reason, the high-temperature thermal treatment process such as an incineration or a pyrolysis is considered as promising technologies, since it provides a substantial volume reduction. Currently, the fluidized bed incineration is considered as efficient technology for the treatment of radioactive graphite waste. In this study, the fluidized bed incineration condition and the radioisotopes behavior were experimentally investigated by using irradiated graphite waste which has arisen from the decommissioning of Korean Research Reactor 2 (KRR-2).

Novel Technology for Hydrothermal Treatment of NPP Evaporator Concentrates

A novel technology was developed for treatment of evaporator concentrates produced as a result of operation of evaporation devices comprising the main component of special water purification systems of nuclear power plants (NPP). The developed technology includes a hydrothermal (T = 250–300°C and P = 80–120 bar) processing of evaporator concentrates in oxidation medium in order to destruct stable organic complexes of cobalt radionuclides and remove these radionuclides by oxide materials formed during such a processing. The cesium radionuclides contained in evaporator concentrates are removed by a conventional method — through application of one of the developed composite sorbents with ferrocyanides of transition metals used as active agents. Extensive laboratory studies of the processes occurring in evaporator concentrates under hydrothermal conditions were performed. It was shown that hydrothermal oxidation of evaporator concentrates has a number of advantages as compared to traditional oxidation methods (ozonation, photocatalytic, electrochemical and plasma oxidation). A laboratory installation was built for the flow-type hydrothermal oxidation of NPP evaporator concentrates. The obtained experimental results showed good prospects for the developed method application. On the basis of the results obtained, a pilot installation of productivity up to 15 l/hour was developed and built in order to work out the technology of evaporator concentrates hydrothermal treatment. The pilot tests of the hydrothermal technology for evaporator concentrates hydrothermal treatment were performed for 6 months in 2006 at the 1st reactor unit of the Novovoronezhskaya NPP (Voronezh Region, Russia). Optimal technological regimes were determined, and estimations of the economic soundness of the technology were made. The advantages of the presented technology in terms of management of concentrated liquid radioactive wastes (LRW) at nuclear cycle facilities, as compared to other methods applicable for this type of LRW, were demonstrated. Application of the hydrothermal technology in the system of NPP LRW management enables one to reduce substantially the volume of solid radioactive waste sent for final disposal.

Melting Characteristics of the Stainless Steel Generated From the Uranium Conversion Plant

The partition ratio of cerium (Ce) and uranium (U) in the ingot, slag and dust phases has been investigated for the effect of the slag type, slag concentration and basicity in an electric arc melting process. An electric arc furnace (EAF) was used to melt the stainless steel wastes, simulated by uranium oxide and the real wastes from the uranium conversion plant in Korea Atomic Energy Research Institute (KAERI). The composition of the slag former used to capture the contaminants such as uranium, cerium, and cesium during the melt decontamination process generally consisted of silica (SiO2), calcium oxide (CaO) and aluminum oxide (Al2O3). Also, Calcium fluoride (CaF2), nickel oxide (NiO), and ferric oxide (Fe2O3) were added to provide an increase in the slag fluidity and oxidative potential. Cerium was used as a surrogate for the uranium because the thermochemical and physical properties of cerium are very similar to those of uranium. Cerium was removed from the ingot phase to slag phase by up to 99% in this study. The absorption ratio of cerium was increased with an increase of the amount of the slag former. And the maximum removal of cerium occurred when the basicity index of the slag former was 0.82. The natural uranium (UO2) was partitioned from the ingot phase to the slag phase by up to 95%. The absorption of the natural uranium was considerably dependent on the basicity index of the slag former and the composition of the slag former. The optimum condition for the removal of the uranium was about 1.5 for the basicity index and 15wt% of the slag former. According to the increase of the amount of slag former, the absorption of uranium oxide in the slag phase was linearly increased due to an increase of its capacity to capture uranium oxide within the slag phase. Through experiments with various slag formers, we verified that the slag formers containing calcium fluoride (CaF2) and a high amount of silica were more effective for a melt decontamination of stainless steel wastes contaminated with uranium. During the melting tests with stainless steel wastes from the uranium conversion plant (UCP) in KAERI, we found that the results of the uranium decontamination were very similar to those of the uranium oxide from the melting of stimulated metal wastes.

Green Remediation: Enhanced Reductive Dechlorination Using Recycled Rinsewater as Bioremediation Substrate

Enhanced reductive dechlorination (ERD) has rapidly become a remedy of choice for use on chlorinated solvent contamination when site conditions allow. With this approach, solutions of an organic substrate are injected into the affected aquifer to stimulate biological growth and the resultant production of reducing conditions in the target zone. Under the reducing conditions, hydrogen is produced and ultimately replaces chlorine atoms on the contaminant molecule causing sequential dechlorination. Under suitable conditions the process continues until the parent hydrocarbon precursor is produced, such as the complete dechlorination of trichloroethylene (TCE) to ethene. The process is optimized by use of a substrate that maximizes hydrogen production per unit cost. When natural biota are not present to promote the desired degradation, inoculates can be added with the substrate. The in-situ method both reduces cost and accelerates cleanup. Successful applications have been extended from the most common chlorinated compounds perchloroethylene (PCE) and TCE and related products of degradation, to perchlorate, and even explosives such as RDX and trinitrotoluene on which nitrates are attacked in lieu of chloride. In recent work, the process has been further improved through use of beverage industry wastewaters that are available at little or no cost. With material cost removed from the equation, applications can maximize the substrate loading without significantly increasing total cost. The extra substrate loading both accelerates reaction rates and extends the period of time over which reducing conditions are maintained. In some cases, the presence of other organic matter in addition to simple sugars provides for longer performance times of individual injections, thereby working in a fashion similar to emulsified vegetable oil. The paper discusses results of applications at three different sites contaminated with chlorinated ethylenes. The applications have included wastewaters of both natural fruit juices and corn syrup solutions from carbonated beverages. Cost implications include both the reduced cost of substrate and the cost avoidance of needing to pay for treatment of the wastewater.

Study of the Oxidation State of Arsenic and Uranium in Individual Particles From Uranium Mine Tailings, Hungary

Uranium ore mining and milling have been terminated in the Mecsek Mountains (southwest Hungary) in 1997. Mine tailings ponds are located between two important water bases, which are resources of the drinking water of the city of Pe´cs and the neighbouring villages. The average U concentration of the tailings material is 71.73 μg/g, but it is inhomogeneous. Some microscopic particles contain orders of magnitude more U than the rest of the tailings material. Other potentially toxic elements are As and Pb of which chemical state is important to estimate mobility, because in mobile form they can risk the water basis and the public health. Individual U-rich particles were selected with solid state nuclear track detector (SSNTD) and after localisation the particles were investigated by synchrotron radiation based microanalytical techniques. The distribution of elements over the particles was studied by micro beam X-ray fluorescence (μ-XRF) and the oxidation state of uranium and arsenic was determined by micro X-ray absorption near edge structure (μ-XANES) spectroscopy. Some of the measured U-rich particles were chosen for studying the heterogeneity with μ-XRF tomography. Arsenic was present mainly in As(V) and uranium in U(VI) form in the original uranium ore particles, but in the mine tailings samples uranium was present mainly in the less mobile U(IV) form. Correlation was found between the oxidation state of As and U in the same analyzed particles. These results suggest that dissolution of uranium is not expected in short term period.