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Modeling of nuclide release from low-level radioactive paraffin waste: a comparison of simulated and real waste.

Nuclide leaching models based on mass transfer theory are reviewed and evaluated to analyze the leaching test results of simulated and real paraffin waste from Korean nuclear power plants (NPPs). An empirical model (EM), bulk diffusion model (BDM), coupled diffusion/dissolution model (CDDM), shrinking core model (SCM), modified SCM (MSCM), and uniform reaction model (URM) are selected for comparison. In case of simulated paraffin waste form, the experimental results are satisfactorily explained by the SCM which is based on a diffusion-controlled dissolution reaction. Leaching behavior of real paraffin waste form is well predicted by URM that considers inter-aggregated porous medium and intra-aggregated porous medium separately. If real paraffin waste forms are manufactured with relatively uniform composition, their leaching behaviors are expected to be similar to those of simulated paraffin waste forms.

Diffusion↗

New efficient calixarene amide ionophores for the selective removal of strontium ion from nuclear waste: synthesis, complexation, and extraction properties.

Three novel lower rim hexamide derivatives 5(6), 7(6), and 9(6) of p-hydroxycalix[6]arene and four octamides 5(8), 7(8)-9(8) derived from the corresponding p-hydroxycalix[8]arene were synthesized, and their potential as extractants in radioactive waste treatment was evaluated, in comparison with upper rim analogues 12(6) and 12(8) and other existing selective neutral ionophores currently used in radioactive waste treatment. Extraction of alkali and alkaline earth metal picrates from water to dichloromethane, and of the corresponding nitrates from acidic water solution simulating radioactive waste, to 2-nitrophenyl hexyl ether (NPHE), showed that the lower rim amides extract divalent cations much better than monovalent ones. The upper rim hexa-12(6) and octamide 12(8) are very inefficient ligands, hardly extracting any cation. In all cases, p-alkoxy octamides are more efficient and selective extractants than the corresponding hexamides. In the case of simulated waste solutions, the distribution coefficients for strontium removal by octamides (6.5 < D(Sr) < 30) are much higher than the corresponding value (D(Sr)) found for dicyclohexyl-18-crown-6 (DC18C6), and the same applies for the strontium/sodium selectivity, which is 6500 < D(Sr)/D(Na) < 30 000 for octamides and 47 for DC18C6. ESI-MS, UV-vis, and X-ray crystal structure studies give consistent results and indicate the formation of 2:1 (cation/ligand) strontium complexes for all octamides tested. Stability constants were determined in homogeneous methanol solution for alkali metal (log beta(11) < or = 2), calcium (4.3 < or = log beta(11) < or = 6.0; 9.4 < or = log beta(21) < or = 12.0), and strontium (5.6 < or = log beta(11) < or = 12.3) ions using a UV-vis competition method with 1-(2-pyridylazo)-2-naphthol (PAN). They confirm the high efficiency and high divalent/monovalent selectivity found in metal ion extraction experiments for the new octamide ligands. Evidence for a positive cooperative effect between the two metal ion binding sites was obtained in the case of the Ca(2+) complex of octamide 1(8).

Journal Article↗

Catalytic oxidation of mixed wastes containing high organic content--emission reduction and the effect of steam.

To resolve mixed organic and radioactive waste disposal problems, Lawrence Berkeley National Laboratory (LBNL) initiated a treatability study using the catalytic chemical oxidation (CCO) system to oxidize a mixed-waste stream and to confine tritium as part of LBNL's pollution prevention program. LBNL has also adopted a legal approach by seeking an equivalent waste-treatment determination for the CCO process, and by petitioning the United States Environmental Protection Agency (EPA) to delist F-coded treatment residues. The results of this study demonstrate that (1) the CCO process can treat aqueous wastes containing a broad range of organic chemicals and achieve more than 99.999% destruction efficiency; (2) greater than 99.9% trapping efficiency for tritiated water can be achieved using an emission-reduction system that also confines the vapor of hydrochloric acid or nitric acid to the liquid residue; and (3) neutralized treatment residues can be disposed of as low-level radioactive waste at a permitted facility after EPA has approved LBNL's petitions, or the tritium in the residues can be recycled. The high oxidation efficiency of the CCO process is mainly due to the optimized operating conditions of the CCO process and the combined effect of steam reforming in the oxidation cell and the catalytic oxidation of organic mixtures and CO in the Pt/Al2O3 catalyst bed.

Catalysis↗

Reference biospheres for post-closure performance assessment: inter-comparison of SHETRAN simulations and BIOMASS results.

Example Reference Biosphere 2B (ERB2B) is a hypothetical river catchment, described in the IAEA-sponsored BIOMASS study on biosphere aspects of post-closure radiological safety assessments for repositories for solid radioactive wastes. In ERB2B, a radioactively contaminated aquifer interacts with the soils and sediments of the river catchment. A 'semi-distributed', lumped-parameter model (SDLP) was set up for the site as part of the BIOMASS study. In the model, empirically derived transfer functions are used to reduce the complexity of real hydrological transport systems to readily calculable mass-balance accounting routines. In this work, a physically based, spatially distributed modelling system SHETRAN was set up for the site and comparison made with the existing SDLP model. The work has shown that, using standard soil properties in SHETRAN, the soil rapidly saturates and much of the hydrologically effective rainfall (precipitation less evapotranspiration) is lost as saturation-excess surface runoff. This is contrary to the assumptions in the SDLP model. The difficulty arose from the original formulation of catchment characteristics in BIOMASS. Specifically, there was a large water volume entering the soils from precipitation together with an upward flux of groundwater across the lower boundary of a substantial part of the catchment. This water had to be lost from the catchment in some way and the thinness of the soil zone precluded dominance of subsurface, lateral flow over surface runoff. Increasing the saturated conductivity from 1 to 20 m d(-1) reduced the surface flows to similar values to those assumed in the SDLP model (this could also have been achieved by increasing the soil depth). Even with the high saturated conductivity there were still major differences between the two representations. In the woodland on the upper slopes of the valley, the SHETRAN simulation was slightly wetter than the SDLP model, whereas in the shrubland and marshland near the river it was drier than the SDLP model. In the SDLP model, subsurface lateral flows are ignored if there is surface flow, and deep subsurface flows are ignored if there are shallow subsurface flows. In the SDLP model, there is a major assumed change in flow regime between summer and winter. This is not the case in the SHETRAN simulation. Overall, this work illustrates the problems of using 'semi-distributed', lumped-parameter models without prior calibration against a physically based model and the potential for implying unexpected and possibly implausible hydrological characteristics through the specification of flows without considering whether they could occur for realistic soil depths and properties. As there is a need for application of such SDLP models, particularly when undertaking probabilistic calculations, it is suggested that, in future, explicit hydrological modelling should be undertaken first, so that a physically realistic representation can be produced as a basis for assessment studies of the migration of radionuclides or other contaminants.

Fresh Water↗

Nuclear waste: increasing scale and sociopolitical impacts.

The article argues that insufficient attention has been paid to the operational aspects of the U.S. radioactive waste management system when it grows to the scale necessary to handle wastes produced by a fully deployed plutonium economy. Without such information, many of the unsettling speculations which have become part of the public debate and are summarized herein cannot be clearly addressed. The article then outlines the types of information necessary to begin estimating the costs and consequences of radioactive waste management. Finally, an index of social exposure to radioactive hazard is proposed to improve the basis for policy decisions in this area.

Economics↗

Development of processes for environmental protection based on self-propagating reactions.

The possibility of exploiting self-propagating reactions for environmental protection is discussed in this paper. In particular, results obtained at the laboratory scale and related to the fixation and consolidation of high level radioactive wastes, the recycling of silicon sludge and aluminum dross produced by semiconductor industries and aluminum foundries, the treating and recycling of a highly toxic solid waste from electrolytic zinc plants, and the degradation of chlorinated aromatics, are examined with particular emphasis on the latter case. Specifically, the self-propagating destruction of hexachlorobenzene and 2-(2-4-dichlorophenoxy)-propanoic acid with calcium hydride as reductive substrate is demonstrated. In fact, the heat liberated by the reactions involved is large enough to guarantee the self-sustaining character of the process within a wide range of reactants compositions. Moreover, no residual chlorinated organic compounds were found in the final solid product. Some reactor engineering aspects, as well as other significant future scientific and technological issues, are also addressed in view of large-scale applicability of processes based on self-propagating reactions. To date, the batch reactor technology seems to be more easily applicable, although the use of continuous reactors is not excluded in the next future.

2,4-Dichlorophenoxyacetic Acid↗

The uptake and distribution of buried radionuclides by pocket gophers (Thomomys bottae).

Material Disposal Area G (Area G) at the Los Alamos National Laboratory is a low-level radioactive waste disposal facility. The noticeably high activity of pocket gophers on closed waste burial sites of various types at Area G resulted in the need to understand possible interactions between gophers and radioactive waste. Fossorial animals can influence the fate of contaminants by directly burrowing into waste trenches, pushing contaminated soil to the surface, or through indirect mechanisms such as consumption of contaminant-laden vegetation or the ingestion of soil. In our study, pocket gophers, mound soil, surface soil, and vegetation were collected at Area G and at offsite reference locations. The samples were analyzed for 241Am, 238Pu, 239Pu, 3H, and total U. It did not appear that gophers were responsible for any upward transport of radionuclides. Concentrations of 241Am, 238Pu, 239Pu, and 3H in some gophers, soil, and vegetation were higher than at reference sites; however, only 3H in gopher carcasses at only one of five sites within Area G was higher than a conservative ecological screening level.

Animals↗

[A questionnaire about radiation safety management of the draining-water system at nuclear medicine facilities].

We conducted a questionnaire survey about radiation-safety management condition in Japanese nuclear medicine facilities to make materials of proposition for more reasonable management of medical radioactive waste. We distributed a questionnaire to institutions equipped with Nuclear Medicine facilities. Of 1,125 institutions, 642 institutes (52.8%) returned effective answers. The questionnaire covered the following areas: 1) scale of an institution, 2) presence of enforcement of radiotherapy, 3) system of a tank, 4) size and number of each tank, 5) a form of draining-water system, 6) a displacement in a radioactive rays management area, 7) a measurement method of the concentration of medical radioactive waste in draining water system, 8) planned and used quantity of radioisotopes for medical examination and treatment, 9) an average displacement of hospital for one month. In most institutions, a ratio of dose limitation of radioisotope in draining-water system was less than 1.0, defined as an upper limitation in ordinance. In 499 hospitals without facilities of hospitalization for unsealed radioisotope therapy, 473 hospitals reported that sum of ratios of dose limits in a draining-water system was less than 1.0. It was calculated by used dose of radioisotope and monthly displacement from hospital, on the premise that all used radioisotope entered in the general draining-water system. When a drainage including radioactivity from a controlled area join with that from other area before it flows out of a institution, it may be diluted and its radioactive concentration should be less than its upper limitation defined in the rule. Especially, in all institutions with a monthly displacement of more than 25,000 m3, the sum of ratio of the concentration of each radionuclide to the concentration limit dose calculated by used dose of radioisotope, indicated less than 1.0.

Humans↗

Reflections on the benefits of participating in ACURI.

There are many benefits to participating in the activities of a low-level radioactive waste generators group. Among them are the sharing of ideas, experience, and successes; ready access to information on all aspects of radioactive waste disposal; and the ability to have input into the regulatory and decision making processes.

Health Physics↗

[The role of Japan Radioisotope Association in nuclear medicine].

The Japan Radioisotope Association (JRIA) is established as a nonprofit organization operated by the users with the purpose of facilitating the utilization of RI. Its major activities include academic activities, supplying RI, labeled compounds and radiopharmaceuticals, and collecting and treating radioactive wastes. All RI, 90% of which is radiopharmaceuticals, are distributed through JRIA. The growing rate of radiopharmaceuticals is now getting slow, and RIA has a tendency to be replaced by nonradioactive assays. Nishina Memorial Cyclotron Center is to be operated for cooperative research projects of all institutions in Japan. Kaya Memorial Takizawa Laboratory is established to treat all medical radioactive wastes.

Japan↗

Specific association of 36Cl with low molecular weight humic substances in soils.

Soils initially contaminated with 36Cl in the chloride form were subjected to solid-liquid extractions using a variety of reagents including deionised water and 1 M sodium hydroxide (NaOH). 1 M NaOH was found to result in the greatest recovery of 36Cl from the soils, a result which provided initial evidence that radioactive chlorine became attached to humic substances present naturally within the soils. Deionised water and 1 M NaOH extracts were subjected to analysis involving separation by gel filtration chromatography (GFC). It was found that 36Cl in 1 M NaOH extracts associated preferentially with low molecular weight (LMW) fractions of humic substances whereas, in deionised water extracts, 36Cl appeared to be present exclusively in the chloride form. Previous literature evidence, mainly from highly organic forest soils, suggests that conversion of stable chlorine from chloride to organic forms can occur as a result of biological action. The present paper also presents good evidence for the specific attachment of stable chlorine (37Cl) to a LMW humic fraction, again demonstrated using GFC separation. Current risk assessments of the deep geological disposal of solid radioactive wastes containing 36Cl typically assume a very low degree of sorption based on the notion that the predominant environmental species of radiochlorine is chloride. This paper concludes with a brief discussion on the implications of organochlorine formation in the biosphere for assessment of the radiological impact of deep geological disposal of solid radioactive wastes.

Adsorption↗

International Arctic Seas Assessment Project.

The International Atomic Energy Agency responded to the news that the former Soviet Union had dumped radioactive wastes in the shallow waters of the Arctic Seas, by launching the International Arctic Seas Assessment Project in 1993. The project had two objectives: to assess the risks to human health and to the environment associated with the radioactive wastes dumped in the Kara and Barents Seas; and to examine possible remedial actions related to the dumped wastes and to advise on whether they are necessary and justified. The current radiological situation in the Arctic waters was examined to assess whether there is any evidence for releases from the dumped waste. Potential future releases from the dumped wastes were predicted, concentrating on the high-level waste objects containing the major part of the radionuclide inventory of the wastes. Environmental transport of released radionuclides was modelled and the associated radiological impact on humans and the biota was assessed. The feasibility, costs and benefits of possible remedial measures applied to a selected high-level waste object were examined. Releases from identified dumped objects were found to be small and localised to the immediate vicinity of the dumping sites. Projected future annual doses to members of the public in typical local population groups were very small, less than 1 microSv--corresponding to a trivial risk. Projected future doses to a hypothetical group of military personnel patrolling the foreshore of the fjords in which wastes have been dumped were higher, up to 4 mSv/year, which still is of the same order as the average annual natural background dose. Moreover, since any of the proposed remedial actions were estimated to cost several million US$ to implement, remediation was not considered justified on the basis of potentially removing a collective dose of 10 man Sv. Doses calculated to marine fauna were insignificant, orders of magnitude below those at which detrimental effects on fauna populations might be expected to occur. Remediation was thus concluded not to be warranted on radiological grounds.

Animals↗

On intergenerational equity and its clash with intragenerational equity and on the need for policies to guide the regulation of disposal of wastes and other activities posing very long-term risks.

This article begins with some history of the derivation of 40 CFR Part 191, the U.S. Environmental Protection Agency (EPA) standard that governs the geologic disposal of spent nuclear fuel and high-level and transuranic radioactive wastes. This is followed by criticisms of the standard that were made by a Sub-Committee of the EPA Science Advisory Board, by the staff of the U.S. Nuclear Regulatory Commission, and by a panel of the National Academies of Science and Engineering. The large disparity in the EPA approaches to regulation of disposal of radioactive wastes and disposal of hazardous, long-lived, nonradioactive chemical waste is illustrated. An examination of the intertwined matters of intergenerational equity and the discounting of future health effects follows, together with a discussion of the conflict between intergenerational equity and intragenerational equity. Finally, issues related to assumptions in the regulations concerning the future state of society and the biosphere are treated, as is the absence of any national philosophy or guiding policy for how to deal with societal activities that pose very long-term risks.

History, 20th Century↗

[Radioactivity in dismantling a betatron].

The authors report on the specific radioactivity of construction components of a 42 MeV betatron measured 28 days after the last run by means of a Ge spectrometer (ultra-pure germanium detector employed in a semiconductor spectroscopic method) recording the gamma spectra of various components of the betatron. This examination served to find out which components would have to be considered as radioactive waste requiring special treatment in accordance with Federal German legislation on radioactive waste disposal (section 47 of the Radiation Protection Ordinance). The examination showed that such special treatment would be required only for the target (main material: platinum) and the Platness-filter (chief constituent: lead) of the decommissioned electron accelerator.

Humans↗

Environment and biology of the Kara Sea: a general view for contamination studies.

The recent revelation that over the past 30 years there has been a history of dumping waste including high-level radioactive wastes in the shallow Kara Sea has caused wide-spread concern. The potential impact of these contaminants and other non-nuclear pollutants in the Arctic ecosystem and on human health need to be assessed and, thus, a better insight gained on radioecological processes in cold waters. The present paper proposes a general view on the biology and the environment of the Kara Sea, as a basic tool for the experimental and modelling assessments of the impact of these contaminants.

Animals↗

The voluntary siting process, a case study in New Jersey.

The Low-Level Radioactive Waste Policy Act of 1980 and its 1985 Amendments has not provided new disposal capacity within the United States; however, sufficient disposal capacity currently exists to handle today's disposal needs. Politics, opposition groups, and public mistrust in government have combined to limit the possibilities for establishing new disposal facilities. In 2000, New Jersey (NJ and Connecticut (CT), as members of the Northeast Compact for the disposal of low-level radioactive waste, admitted South Carolina (SC) to their compact, renaming it as the "Atlantic Compact." The advantage to SC is that they are able to prevent disposal of waste from outside the Compact. The advantage to NJ and CT is that they are guaranteed waste disposal for approximately the next 50 years, or until all currently operating nuclear power plants in the states are decommissioned. This paper details the process, much of it not following the scientific method, to try to site a low-level waste facility in NJ. With the formation of the NJ Siting Board in 1987, an effort was made to locate a site using deterministic criteria; however, in 1992, the Board shifted to a voluntary process. In 1998, the Board made the determination that there was adequate capacity for waste disposal and ended active siting. In 2000, the opportunity to form the Atlantic Compact ended siting through an out-of-state solution. While it is not clear that the voluntary process would have ultimately worked in NJ, it has worked in Canada and the process may be one of the few mechanisms for the siting of any type of hazardous material disposal facility. Also, other states still have to decide what they will do after 2008 when Barnwell is no longer open to them.

Clinical Trials Data Monitoring Committees↗