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Environmental biochemistry of current environmental levels of heavy metals: preparation of radiotracers with very high specific radioactivity for metallobiochemical experiments on laboratory animals.

Environmental toxicology research on dose-response relationships of heavy metals requires experiments on laboratory animals exposed to "low doses" of trace elements which should reflect "present or actual environmental levels" characteristic of polluted environments. Unfortunately no criteria exist to establish the "low doses" to which laboratory animals must be exposed, in practice the choice of the level used is made in an almost arbitrary manner. In order to define the "present environmental levels" of heavy metals which should be administered to laboratory animals an approach is suggested, based upon knowledge of the concentrations of trace elements in the diet, air and food as well as the fractions absorbed. Today daily intakes of trace elements by man are of the order of few micrograms or nanograms thus requiring the use of extremely sensitive analytical techniques to determine the very low amounts of heavy metals in tissues and cellular components. In these fields of research the use of radiotracers with very high specific radioactivity appears particularly advantageous but requires considerable care during their preparation and use. The first part of this paper deals with a definition of the ranges of concentrations of trace elements which should be used for metabolic studies on laboratory animals when they are exposed via different routes such as ingestion, inhalation in injection; the second part describes the production of radiotracers with very high specific radioactivity by proton activation in the cyclotron and by neutron irradiation in the nuclear reactor. Their use to label present levels of heavy metals under conditions adapted for biochemical purposes, as well as the preparation of different metal-labelled chemical species is also reported. Particular attention is directed to quality control of the radiotracer solutions which are administered to the animals including those of radioactivity concentrations, radioisotopic purity, radiochemical purity, carrier content and chemical impurities.

Animals↗

Radioactivity in the Great Lakes.

Studies of radioactivity in the Laurentian Great Lakes are reviewed to evaluate the impact of radionuclide dissemination on the world's foremost freshwater aquatic ecosystem. The status of radiologically-degraded areas is also reported. Significant amounts of radioactivity are stored in the basin, which has numerous nuclear reactors as well as uranium mine waste areas. The prevailing low levels of artificially-produced radionuclides, arising largely from previous fallout inputs, provide very little radiation dose to the area residents consuming lake water. The interlake transport of radionuclides is adequately described by existing models, though some refinement of the source term is needed. Revised estimates of fallout over each lake are given, but no data are available to estimate drainage basin contributions. Only limited information is available on the dispersal of radioactive pollutants. The influence of chemical parameters on radionuclide cycling has been extensively investigated in Lake Michigan and, to a lesser degree, in Lake Ontario. The need for developing a radiological objective for fish becomes apparent from an assessment of the very few data collected thus far on the biological and dosimetric aspects. Several research and monitoring needs are also identified.

Canada↗

Investigation of lead radioactivity.

Surface alpha radioactivity of lead after surface rescraping increases with time approximately exponentially, with a relaxation time of a few days. Increment of the alpha radioactivity is comparable with initial radioactivity after rescraping. Hypothesis of the atomic mechanism of this effect is presented.

Alpha Particles↗

Experimental electron beam irradiation of food and the induction of radioactivity.

Samples of chicken, prawns, cheeses and spices were irradiated on the Harwell electron linear accelerator HELIOS at 20 MeV to assess mechanisms for the induction of radioactivity. The induced radioactivity was measured using a lead shielded Ge(Li) gamma-ray spectrometer, and the results were compared with activities calculated on the basis of photoneutron and photoproton reactions induced by real and virtual photons. In general, there was good agreement. Bounds were also placed on the induction of radioactivity by capture of neutrons produced in the food samples themselves. Further, the data were used to assess the effects of a gross malfunction of an electron beam irradiation facility; after 1 day, the specific activity of food samples irradiated to 10 kGy at 20 MeV was approximately 0.01 Bq g-1. In addition, food samples were also irradiated at 10 MeV, and irradiated and control samples were analysed for microbiological burden. Reductions in the microbiological burden of the food samples by factors consistent with those found in previous measurements were found.

Electrons↗

Radioactive iodine waste treatment using electrodialysis with an anion exchange paper membrane.

In order to simply and safely treat radioactive iodine waste, a study of the removal of iodide ion from radioactive waste using electrodialysis with an anion exchange paper membrane, in which trimethylhydroxylpropylammonium groups were homogeneously dispersed with high density. In Na125I and Na36Cl concentration-cell system, electric ion and water conductances, phenomenological coefficients, have been experimentally determined on basis of nonequilibrium thermodynamics. Prepared paper membrane had higher permselectivity of 125I ion than 36Cl ions by approximately 21%. On the other hand, water flux that was accompanied by an ionic transference in prepared paper membrane was greatly larger than that in typical synthesized membrane. It is suggested that a depression of water mobility is important to practice an ideal radioactive iodide waste electrodialysis system with a novel anion exchange paper membrane.

Anions↗

Identification of radioactive materials in moving objects.

Control over the transportation of the radioactive materials crossing the borders of Uzbekistan is actually today not like before, because of increased threat of terrorism and urges of terrorist organizations to use radioactive materials in their terrorist activities. There are many companies producing radiation control systems. All such systems existing nowadays are based on the principles of intensity comparison for radiation detected by the system in the absence of control object and the intensity of the radiation when object appears. This method works well only in the conditions of constant or weakly changing background. However, at significant deviation in the value of background the number of false alarms set off by the systems increases. The present work describes the method for radioactive materials detection in the moving objects independent of the significant background deviations and present radiation monitoring establishment based on this principle.

Elements, Radioactive↗

Pollution of the Begej Canal sediment--metals, radioactivity and toxicity assessment.

The Begej Canal is one among a large number of canals in Vojvodina (Northern Province of Serbia and Montenegro). The paper describes a study of metal and radioactivity contamination of the Begej Canal sediment. It is also concerned with the evaluation of sediment acute toxicity based on standard test species Daphnia magna and simultaneously extracted metals and acid volatile sulfides. The quality of sediment was assessed according to Dutch standards, but the results were also compared with some Canadian and USEPA (United States Environmental Protection Agency) guidelines for sediment quality. The results showed severe pollution with chromium, copper, cadmium and zinc, whereby the anthropogenic origin of these contaminants was indicated. The tests of toxicity of sediment pore water to D. magna, gave no indication of the presence of substances in acutely toxic concentrations to this species. It can be speculated that, despite of high metal contents, the observed toxicity was low because of the high contents of clay and iron, as well as sulphide. Also, based on a comparison with the Danube sediment and Vojvodina soil in general, the data of the Begej sediment contamination with 238U and 137Cs. The 137Cs data were used for approximate dating of the sediment. No traces of contamination by nuclear power plants in the region were found, while the presence of technologically enhanced naturally occurring radioactive materials (TENORM) was proved. Conclusions based on different criteria for sediment quality assessment were in some cases contradictory. Study also showed that radioactivity aspects can be useful in sediment quality surveys. The obtained results will be invaluable for the future activities regarding integrated water management based on EC Water Framework Directive (2000/60/EC) in the Danube basin, and particularly in the region of crossborder water body of the Begej Canal.

Animals↗

Occupational exposure of phosphate mine workers: airborne radioactivity measurements and dose assessment.

Under the Egyptian program for radiation safety and control, airborne radioactivity measurements and radiological dose assessment were conducted in some phosphate and uranium mines. Abu-Tartor mine is one of the biggest underground phosphate mines in Egypt. Airborne radioactivity, radon ((222)Rn) and its short-lived decay products (progenies) and thoron ((220)Rn), were measured in selected locations along the mine. The environmental gamma and workers dose equivalent rate (mSv/y) were measured inside and outside the mine using thermo-luminescence dosimeters (TLD). The results were presented and discussed. The calculated annual effective dose due to airborne radioactivity is the main source of occupational exposure and exceeding the maximum recommended level by ICRP-60 inside the mine tunnels. A number of recommendations are suggested to control the occupational exposures.

Air Pollutants, Radioactive↗

Radioactivity of the soil in Vojvodina (northern province of Serbia and Montenegro).

The widespread public belief that during the bombardment of Vojvodina (Yugoslavia) this region was contaminated by depleted uranium has recently raised public concern with respect to the potential contamination of agricultural products due to soil radioactivity. Based on the gamma-spectrometric analysis of 50 soil samples taken from the region of Vojvodina we concluded that there is no increase of radioactivity that could endanger the food production. Taking into account the transfer factors of 137Cs to plants, the measured activity concentrations of this isotope should not endanger the health safety of the produced food. No traces of depleted uranium have been found. The natural radioactivity levels are compared with the results form other countries.

Cesium Radioisotopes↗

Comparative assessment of natural radioactivity in fallout samples from Patras and Megalopolis, Greece.

Bulk deposition samples were collected simultaneously from two Greek cities, Patras and Megalopolis, with different emission sources of natural radioactivity, on a monthly basis, during a whole year. Gross beta-activity and 238U- and 232Th-activities were determined in a total of 95 samples of deposited dust. The results were statistically analyzed in order to determine the natural radioactivity levels and their variations in the above cities. No significant difference was found in deposited dust amount between the two cities, while the values of gross beta-, 238U- and 232Th-activities were about 3, 71 and 4 times higher in Megalopolis than in Patras, respectively. This was attributed to the operation of lignite power plants A and B in the vicinity of the city of Megalopolis, while natural radioactivity concentrations in Patras' fallout samples were of natural sources.

Carbon↗

The source of anomalous radioactivity in the springs bordering the Sea of Galilee, Israel.

Situated within the Jordan Rift Valley, along the shores of Lake Kinneret (Sea of Galilee) which serves as the national water reservoir of Israel, are saline hot springs that are notable for their enrichment in radon and radium. Though the anomalous radioactivity has been known for almost half a century, the source of the radioactive anomalies has been a subject of conjecture. Radiometric analysis of a rock core drilled through Mt. Arbel, situated to the west of the lake, reveals that the oil shale sequence of the Senonian En Zetim and Ghareb formations is strikingly deficient in radium. Mt. Arbel has been cut by Rift Valley related faults that serve as conduits for ascending brines. The organic matter enriched sequence is encountered in the subsurface at elevations lower than the water level of the nearby radioactive enriched hot springs. It is thus concluded that hot ascending brines underlying the lake flush through the organic matter enriched sequence and remove a substantial percentage of 226Ra from the uranium enriched organic material, before draining to the outlets of the springs. Saline springs that are in contact with organic matter enriched sequence show excess of radium and radon, while fresh water springs in the same stratigraphic position show only excess of radon.

Israel↗

Advances in cement solidification technology for waste radioactive ion exchange resins: a review.

Treatment and disposal of waste radioactive ion exchange resins is one of the most urgent problems for nuclear industries in China. Cement solidification technology has many advantages, such as requiring simple equipment, easy scaling-up, low working temperature, no trouble of gas cleaning and low cost. It is a suitable technology for treatment of waste radioactive resins, and has been widely used. The new developments and theoretical basis of cement solidification of radioactive resins were introduced in this paper. The cement solidification technology suitable for China and the questions needed to solve were also discussed.

Hot Temperature↗

Treatment of radioactive liquid waste by sorption on natural zeolite in Turkey.

Liquid radioactive waste has been generated from the use of radioactive materials in industrial applications, research and medicine in Turkey. Natural zeolites (clinoptilolite) have been studied for the removal of several key radionuclides ((137)Cs, (60)Co, (90)Sr and (110m)Ag) from liquid radioactive waste. The aim of the present study is to investigate effectiveness of zeolite treatment on decontamination factor (DF) in a combined process (chemical precipitation and adsorption) at the laboratory tests and scale up to the waste treatment plant. In this study, sorption and precipitation techniques were adapted to decontamination of liquid low level waste (LLW). Effective decontamination was achieved when sorbents are used during the chemical precipitation. Natural zeolite samples were taken from different zeolite formations in Turkey. Comparison of the ion-exchange properties of zeolite minerals from different formations shows that Gordes clinoptilolite was the most suitable natural sorbent for radionuclides under dynamic treatment conditions and as an additive for chemical precipitation process. Clinoptilolite were shown to have a high selectivity for (137)Cs and (110m)Ag as sorbent. In the absence of potassium ions, native clinoptilolite removed (60)Co and (90)Sr very effectively from the liquid waste. In the end of this liquid waste treatment, decontamination factor was provided as 430 by using 0.5 mm clinoptilolite at 30 degrees C.

Adsorption↗

Synthesis of a radioactive thiol reagent, 1-S-[3H]carboxymethyl-dithiothreitol: identification of the phosphorylation sites by N-terminal peptide sequencing and matrix-assisted laser desorption/ionization time-of-flight mass spectrometry.

A novel radioactive thiol reagent, 1-S-[3H]carboxymethyl-dithiothreitol (DTT-S-C[3H(2)]CO(2)H, [3H]CM-DTT), was designed and synthesized at the micromole level by reaction of dithiothreitol with tritiated iodoacetic acid (I-C[3H(2)].CO(2)H). The reaction progress was followed by reverse-phase high-performance liquid chromatography (RP-HPLC) and matrix-assisted laser desorption/ionization time-of-flight mass spectrometry. The usefulness of the synthesized reagent was evaluated in a series of experimental approaches. (i) The synthetic phosphopeptide, NSVS(P)EEGRGDSV, was derivatized by [3H]CM-DTT separated from excess reagent by RP-HPLC. The extent of derivatization was quantitated in terms of the mol of P-Ser/mol of peptide by 3H counting, and the location of the phosphoserine was defined by the N-terminal Edman degradation sequence analysis as being the fourth amino acid residue from the N terminus. (ii) A sample of trypsin-digested alpha-casein was derivatized with [3H]CM-DTT, peptides were separated by RP-HPLC, and aliquots of each fraction were counted for 3H label within the peptide map which rapidly pinpointed the original four phosphoserine-containing peptides. This demonstrated the utility of the synthesized radioactive thiol agent in rapid purification and identification of phosphopeptides from HPLC peptide mapping of proteolytic digests of phosphoproteins. (iii) The [3H]CM-DTT was also used to determine the extent of phosphorylation of phosphoproteins both qualitatively by sodium dodecyl sulfate-polyacrylamide gel electrophoresis and autoradiography and quantitatively by 3H counting. The synthesized radioactive thiol reagent [3H]CM-DTT proved to be very efficient and sensitive and should be adaptable to a wide range of routinely utilized laboratory approaches in many fields of the biological sciences.

Binding Sites↗

Prediction of the fate of radioactive material in the South Pacific Ocean using a global high-resolution ocean model.

We investigate the release of radioactive contaminants from Moruroa Atoll in a global high-resolution off-line model. The spread of tracer is studied in a series of simulations with varying release depths and time-scales, and into ocean velocity fields corresponding to long-term annual mean, seasonal, and interannually varying scenarios. In the instantaneous surface release scenarios we find that the incorporation of a seasonal cycle greatly influences tracer advection, with maximum concentrations still found within the French Polynesia region after 10 years. In contrast, the maximum trace is located in the southeast Pacific when long-term annual mean fields are used. This emphasizes the importance of the seasonal cycle in models of pollution dispersion on large scales. We further find that during an El Niño/Southern Oscillation (ENSO) event reduced currents in the region of Moruroa Atoll result in increased concentrations of radioactive material in French Polynesia, as direct flushing from the source is reduced. In terms of the sensitivity to tracer release time-rates, we find that a gradual input results in maximum concentrations in the near vicinity of French Polynesia. This contrasts the instantaneous-release scenarios, which see maximum concentrations and tracer spread across much of the South Pacific Ocean. For example, in as little as seven years radioactive contamination can reach the east coast of Australia diluted by only a factor of 1,000 of the initial concentration. A comparison of results is made with previous studies. Overall, we find much higher concentrations of radionuclides in the South Pacific than has previously been predicted using coarser-resolution models.

Forecasting↗

Radioactivity in bottled mineral waters.

Consumption of bottled mineral water is a growing practice and is sometimes a necessity rather than a choice. In this work, a study of the radioactive content of a wide selection of commercial bottled mineral waters for human intake was carried out. The origins of the analyzed waters were very different, coming from various locations in France, Portugal and Spain. Their total alpha and beta activity concentrations were determined and also gamma spectrometry was used to detect some radionuclides. In some cases, the waters presented high values of the total alpha and beta activity concentrations surpassing the reference levels established by the CSN, the Spanish. Regulatory Organization. In these cases, a determination of uranium and 226Ra was also performed by using low-level liquid scintillation counting. The results revealed a strong correlation between radioactive content and dry residue, and lead one to conclude that high radioactive content is mainly related to the mineralization in waters of underground origin.

Alpha Particles↗

On-line liquid chromatography-accurate radioisotope counting coupled with a radioactivity detector and mass spectrometer for metabolite identification in drug discovery and development.

A novel detection method combining on-line liquid chromatography-accurate radioisotope counting (LC-ARC, advanced stop flow controller) coupled with a radioactivity detector and mass spectrometer has been developed. One of the major benefits of this method is that this system enhances the sensitivity of radioisotope measurement for metabolite identification in drug metabolism studies. Another advantage to this system is the easy interface with the mass spectrometer, which allows acquisition of mass spectrometric data on-line. For purposes of evaluating this system, in vitro microsomal incubations with [3Hlpropranolol were conducted. On-line separation and identification of [3H]propranolol metabolites was achieved without intensive sample preparation, concentration, or fraction collection. Mass spectrometric analysis showed the presence of propranolol major metabolites formed by hydroxylation, correlating with previously published results. Further evaluations of this system also were conducted using two 14C compounds, which are herein labeled X and Y. As our results show, 14C peaks were detected down to 6 cpm, which is approximately 20 times more sensitive than commercially available flow through radioactivity detectors. The overall results suggest that the combination of LC-ARC with radioactivity detection and mass spectrometry has great potential as a powerful tool for improving the sensitivity of radioisotope measurement in metabolite identification studies during drug discovery and development.

Animals↗

Foaming in simulated radioactive waste.

Radioactive waste treatment process usually involves concentration of radionuclides before waste can be immobilized by storing it in stable solid form. Foaming is observed at various stages of waste processing like SRAT (sludge receipt and adjustment tank) and melter operations. This kind of foaming greatly limits the process efficiency. The foam encountered can be characterized as a three-phase foam that incorporates finely divided solids (colloidal particles). The solid particles stabilize foaminess in two ways: by adsorption of biphilic particles at the surfaces of foam lamella and by layering of particles trapped inside the foam lamella. During bubble generation and rise, solid particles organize themselves into a layered structure due to confinement inside the foam lamella, and this structure provides a barrier against the coalescence of the bubbles, thereby causing foaming. Our novel capillary force balance apparatus was used to examine the particle-particle interactions, which affect particle layer formation in the foam lamella. Moreover, foaminess shows a maximum with increasing solid particle concentration. To explain the maximum in foaminess, a study was carried out on the simulated sludge, a non-radioactive simulant of the radioactive waste sludge at SRS, to identify the parameters that affect the foaming in a system characterized by the absence of surface-active agents. This three-phase foam does not show any foam stability unlike surfactant-stabilized foam. The parameters investigated were solid particle concentration, heating flux, and electrolyte concentration. The maximum in foaminess was found to be a net result of two countereffects that arise due to particle-particle interactions: structural stabilization and depletion destabilization. It was found that higher electrolyte concentration causes a reduction in foaminess and leads to a smaller bubble size. Higher heating fluxes lead to greater foaminess due to an increased rate of foam lamella generation in the sludge system.

Chemical Phenomena↗