Residual radionuclide concentrations and estimated radiation doses at the former French nuclear weapons test sites in Algeria.

In order to assess the level of residual radioactivity and evaluate the radiological conditions at the former French nuclear testing sites of Reggane and Taourirt Tan Afella in the south of Algeria, the International Atomic Energy Agency, at the request of the government of Algeria, conducted a field mission to the sites in 1999. At these locations, France conducted a number of nuclear tests in the early 1960s. At the ground zero locality of the ''Gerboise Blanche'' atmospheric test (Reggane) and in the vicinity of a tunnel where radioactive lava was ejected during a poorly contained explosion (Taourirt Tan Afella), non-negligible levels of radioactive material could still be measured. Using the information collected and using realistic potential exposure scenarios, radiation doses to potential occupants and visitors to the sites were estimated.

Oxidation states of uranium in depleted uranium particles from Kuwait.

The oxidation states of uranium in depleted uranium (DU) particles were determined by synchrotron radiation based mu-XANES, applied to individual particles isolated from selected samples collected at different sites in Kuwait. Based on scanning electron microscopy with X-ray microanalysis prior to mu-XANES, DU particles ranging from submicrons to several hundred micrometers were observed. The median particle size depended on sources and sampling sites; small-sized particles (median 13 microm) were identified in swipes taken from the inside of DU penetrators holes in tanks and in sandy soil collected below DU penetrators, while larger particles (median 44 microm) were associated with fire in a DU ammunition storage facility. Furthermore, the (236)U/(235)U ratios obtained from accelerator mass spectrometry demonstrated that uranium in the DU particles originated from reprocessed fuel (about 10(-2) in DU from the ammunition facility, about 10(-3) for DU in swipes). Compared to well-defined standards, all investigated DU particles were oxidized. Uranium particles collected from swipes were characterized as UO(2), U(3)O(8) or a mixture of these oxidized forms, similar to that observed in DU affected areas in Kosovo. Uranium particles formed during fire in the DU ammunition facility were, however, present as oxidation state +5 and +6, with XANES spectra similar to solid uranyl standards. Environmental or health impact assessments for areas affected by DU munitions should therefore take into account the presence of respiratory UO(2), U(3)O(8) and even UO(3) particles, their corresponding weathering rates and the subsequent mobilisation of U from oxidized DU particles.

Properties, use and health effects of depleted uranium (DU): a general overview.

Depleted uranium (DU), a waste product of uranium enrichment, has several civilian and military applications. It was used as armor-piercing ammunition in international military conflicts and was claimed to contribute to health problems, known as the Gulf War Syndrome and recently as the Balkan Syndrome. This led to renewed efforts to assess the environmental consequences and the health impact of the use of DU. The radiological and chemical properties of DU can be compared to those of natural uranium, which is ubiquitously present in soil at a typical concentration of 3 mg/kg. Natural uranium has the same chemotoxicity, but its radiotoxicity is 60% higher. Due to the low specific radioactivity and the dominance of alpha-radiation no acute risk is attributed to external exposure to DU. The major risk is DU dust, generated when DU ammunition hits hard targets. Depending on aerosol speciation, inhalation may lead to a protracted exposure of the lung and other organs. After deposition on the ground, resuspension can take place if the DU containing particle size is sufficiently small. However, transfer to drinking water or locally produced food has little potential to lead to significant exposures to DU. Since poor solubility of uranium compounds and lack of information on speciation precludes the use of radioecological models for exposure assessment, biomonitoring has to be used for assessing exposed persons. Urine, feces, hair and nails record recent exposures to DU. With the exception of crews of military vehicles having been hit by DU penetrators, no body burdens above the range of values for natural uranium have been found. Therefore, observable health effects are not expected and residual cancer risk estimates have to be based on theoretical considerations. They appear to be very minor for all post-conflict situations, i.e. a fraction of those expected from natural radiation.

Isotopic composition and origin of uranium and plutonium in selected soil samples collected in Kosovo.

Soil samples collected from locations in Kosovo where depleted uranium (DU) ammunition was expended during the 1999 Balkan conflict were analysed for uranium and plutonium isotopes content (234U, 235U, 236U, 238U, 238Pu, (239 + 240)Pu). The analyses were conducted using gamma spectrometry (235U, 238U), alpha spectrometry (238Pu, (239 + 240)Pu), inductively coupled plasma-mass spectrometry (ICP-MS) (234U, 235U, 236U, 238U) and accelerator mass spectrometry (AMS) (236U)). The results indicated that whenever the U concentration exceeded the normal environmental values (approximately 2 to 3 mg/kg) the increase was due to DU contamination. 236U was also present in the released DU at a constant ratio of 236U (mg/kg)/238U (mg/kg) = 2.6 x 10(-5), indicating that the DU used in the ammunition was from a batch that had been irradiated and then reprocessed. The plutonium concentration in the soil (undisturbed) was about 1 Bq/kg and, on the basis of the measured 238Pu/(239 + 240)Pu, could be entirely attributed to the fallout of the nuclear weapon tests of the 1960s (no appreciable contribution from DU).

Depleted uranium particles in selected Kosovo samples.

Selected soil samples, collected in Kosovo locations where DU ammunition was expended during the 1999 Balkan conflict, have been investigated by secondary ion mass spectrometry (SIMS), X-ray fluorescence imaging using a micro-beam (micro-XRF) and scanning electron microscopy equipped with an energy dispersive X-ray fluorescence detector (SEM-EDXRF), with the objective to test the suitability of these techniques to identify the presence of small DU particles and measure their size distribution and the 235U/238U isotopic ratio (SIMS). Although the results do not permit any legitimate extrapolation to all the sites hit by the DU rounds used during the conflict, they indicated that there can be "spots ' where hundreds of thousands of particles may be present in a few milligrams of DU contaminated soil. The particle size distribution showed that most of the DU particles were <5 microm in diameter and more than 50% of the particles had a diameter <1.5 microm. Knowledge on DU particles is needed as a basis for the assessment of the potential environmental and health impacts of military use of DU, since it provides information on possible re-suspension and inhalation.

Oxidation states of uranium in DU particles from Kosovo.

The oxidation states of uranium contained in depleted uranium (DU) particles were determined by synchrotron radiation based micro-XANES, applied to individual particles in soil samples collected at Ceja Mountain, Kosovo. Based on scanning electron microscopy (SEM) with XRMA prior to micro-XANES, DU particles ranging from submicrons to about 30 microm (average size: 2 microm or less) were identified. Compared to well-defined standards, all investigated DU particles were oxidized. About 50% of the DU particles were characterized as UO2, the remaining DU particles present were U3O8 or a mixture of oxidized forms (ca. 2/3 UO2, 1/3 U3O8). Since the particle weathering rate is expected to be higher for U3O8 than for UO2, the presence of respiratory U3O8 and UO2 particles, their corresponding weathering rates and subsequent remobilisation of U from DU particles should be included in the environmental or health impact assessments.

Radioecological survey at selected sites hit by depleted uranium ammunitions during the 1999 Kosovo conflict.

A field study, organised, coordinated and conducted under the responsibility of the United Nations Environment Programme (UNEP), took place in Kosovo in November 2000 to evaluate the level of depleted uranium (DU) released into the environment by the use of DU ammunition during the 1999 conflict. Representatives of six different scientific organisations took part in the mission and a total of approximately 350 samples were collected. During this field mission, the Italian National Environmental Protection Agency (ANPA) collected water, soil, lichen and tree bark samples from different sites. The samples were analysed by alpha-spectroscopy and in some cases by inductively coupled plasma-source mass spectrometry (ICP-MS). The 234U/238U and 235U/238U activity concentration ratios were used to distinguish natural from anthropogenic uranium. This paper reports the results obtained on these samples. All water samples had very low concentrations of uranium (much below the average concentration of drinking water in Europe). The surface soil samples showed a very large variability in uranium activity concentration, namely from approximately 20 Bq kg(-1) (environmental natural uranium) to approximately 2.3 x 10(5) Bq kg(-1) (approximately 18000 mg kg(-1) of depleted uranium), with concentrations above environmental levels always due to DU. The uranium isotope measurements refer to soil samples collected at places where DU ammunition had been fired; this variability indicates that the impact of DU ammunitions is very site-specific, reflecting both the physical conditions at the time of the impact of the DU ammunition and any physical and chemical alteration which occurred since then. The results on tree barks and lichens indicated the presence of DU in all cases, showing their usefulness as sensitive qualitative bio-indicators for the presence of DU dusts or aerosols formed at the time the DU ammunition had hit a hard target. This result is particularly interesting considering that at some sites, which had been hit by DU ammunition, no DU ground contamination could be detected.

Results of the intercalibration study of laboratories involved in assessing the environmental consequences of the Chernobyl accident.

Within the framework of the International Chernobyl Project, the IAEA's Seibersdorf Laboratories organized an intercalibration exercise among some of the laboratories which were involved in assessing the environmental contamination in the USSR due to the accident. The objective was to assess the reliability of the radioanalytical data for food and environmental samples, which were used to assess the doses. In the initial study reference materials from the stocks of the IAEA's Analytical Quality Control Services (AQCS) were re-labelled and submitted to 71 laboratories as blind samples. These natural matrix materials included samples of milk (containing 2 different levels of radioactivity), soil, air filters and clover. The concentrations of radionuclides in these samples were known from previous intercalibration exercises. The overall range in performance was broad, which is similar to what has been observed in previous international intercomparisons. The results obtained by gamma-ray spectrometry tended to be somewhat underestimated, on average. On the other hand, the laboratories showed an overall tendency to overestimate 90Sr and possibly 239Pu, which were analysed radiochemically. The intercalibration exercise is continuing with nine materials, including: soil, grass, hay and milk powder contaminated with fallout from the Chernobyl accident. These materials, which were prepared by laboratories in the USSR, are now being tested by AQCS prior to future intercomparison exercises. Work with these materials is expected to continue for several years.

Liquid membrane potential in nonisothermal systems.

Electrical membrane potential equations for liquid ion exchange membranes, characterized by the presence of uncharged associated species and by exclusion of co-ions (no electrolyte uptake) have been derived. The irreversible thermodynamic theories already developed for solid membranes with fixed charged site density have been extended to include the different physicochemical aspects of the liquid membranes. To this purpose the dissipation function has been written with reference to the fluxes of all the species present in the membrane. It has been found that the mobile charged site, the counterions, and the uncharged associated species contribute to the electrical membrane potential through their phenomenological coefficients. The electrical membrane potential equations have been integrated in isothermal and nonisothermal conditions for monoionic and biionic systems. The theoretical predictions have been experimentally tested by studying the electrical potential of liquid membranes formed with solutions of tetraheptylammonium salts in omicron-dichlorobenzene.