Measurement of transuranic elements,chiefly 237Np (by neutron activation analysis), in the physical and biological compartments of the French shore of the English channel

The behaviour of transuranic elements in the marine environment has been studied via both in situ sampling and laboratory tracer experiments. In particular, the radionuclide ²³⁷Np was investigated and techniques for its quantitative determination are described. In the field investigations, a preliminary separation of Np from samples was performed prior to neutron activation analysis, with subsequent γ-ray spectrometry of ²³⁸Np. In the laboratory studies, ²³⁷Np was determined by a radiochemical method followed by α-spectrometry. The results obtained from the in situ study in the English Channel (sea water, seaweed, molluscs) and from laboratory-uptake experiments (water and mussels) are described. Levels of Pu, Am and Np are compared and the characteristics of neptunium transfer to molluscs are discussed.     

Indoor and outdoor Radon concentration measurements in Sivas, Turkey, in comparison with geological setting

Indoor and soil gas Radon (²²²Rn) concentration measurements were accomplished in two stages in Sivas, a central eastern city in Turkey. In the first stage, CR-39 passive nuclear track detectors supplied by the Turkish Atomic Energy Authority (TAEA) were placed in the selected houses throughout Sivas centrum in two seasons; summer and winter. Before the setup of detectors, a detailed questionnaire form was distributed to the inhabitants of selected houses to investigate construction parameters and properties of the houses, and living conditions of inhabitants. Detectors were collected back two months later and analysed at TAEA laboratories to obtain indoor ²²²Rn gas concentration values. In the second stage, soil gas ²²²Rn measurements were performed using an alphameter near the selected houses for the indoor measurements. Although ²²²Rn concentrations in Sivas were quite low in relation with the allowable limits, they are higher than the average of Turkey. Indoor and soil gas ²²²Rn concentration distribution maps were prepared seperately and these maps were applied onto the surface geological map. In this way, both surveys were correlated with the each other and they were interpreted in comparison with the answers of questionnaire and the geological setting of the Sivas centrum and the vicinity.     

Radioactivity in environmental samples: Calibration standards measurement methods,quality assurance,and data analysis

The numerous environmental radioactivity measurements made by and for the U.S. Environmental Protection Agency (U.S. EPA) include measurements on samples of water, urine, food, milk, and air filters. Calibration standards are listed which are available in the form of water solutions and soils for a wide range of radionuclides. Method validation procedures for U.S. EPA approval include protocol development and single-laboratory and multiple-laboratory evaluation for precision and accuracy. Interlaboratory comparison studies are conducted for both cross-check and performance evaluation samples and involve 295 federal, state, and local laboratories. For water samples, 80%–90% of the participating laboratories are within the control limits for most of the radionuclides measured; however, some problem areas exist, especially for radium-228 and strontium-89 and -90. For milk and food samples, more than 90% of the laboratories are within control limits for cobalt-60 and cesium-137 but some problems exist for the measurement of strontium-90, iodine-131, and potassium-40. For tritium, 91% of the laboratories are within the control limit for water samples and 87% are within the control limits for the urine samples. The laboratory performance for air filter samples shows some problems for gross beta, strontium-90 and cesium-137 measurements.     

Marked disequilibrium between 234Th and 230Th of the 238U natural radioactive decay chain in IAEA reference materials n. 312, 313 and 314

A new laboratory for the spectroscopy of natural radioactivity with a good energy resolution is presented. It consists of two distinct parts equipped, respectively, the first one with a HpGe γ-ray detector, whose setup has been already completed, and the second one with large area Silicon α-ray detectors and a radiochemical section for thin α-samples preparation, whose setup is yet in progress and will be the argument of a separate work.The γ-ray spectrometer was calibrated by means of IAEA Reference Materials n. 312, 313, 314 and 375. A large difference from the predictions of secular equilibrium emerged between the activities of ²³⁴Th and ²³⁰Th in Materials n. 312, 313 and 314.     

Application of in-situ measurement to determine Cs in the Swiss Alps

Establishment of ¹³⁷Cs inventories is often used to gain information on soil stability. The latter is crucial in mountain systems, where ecosystem stability is tightly connected to soil stability. In-situ measurements of ¹³⁷Cs in steep alpine environments are scarce. Most studies have been carried out in arable lands and with Germanium (Ge) detectors. Sodium Iodide (NaI) detector system is an inexpensive and easy to handle field instrument, but its validity on steep alpine environments has not been tested yet. In this study, a comparison of laboratory measurements with GeLi detector and in-situ measurements with NaI detector of ¹³⁷Cs gamma soil radiation has been done in an alpine catchment with high ¹³⁷Cs concentration (Urseren Valley, Switzerland). The aim of this study was to calibrate the in-situ NaI detector system for application on steep alpine slopes. Replicate samples from an altitudinal transect through the Urseren Valley, measured in the laboratory with a GeLi detector, showed a large variability in ¹³⁷Cs activities at a meter scale. This small-scale heterogeneity determined with the GeLi detector is smoothed out by uncollimated in-situ measurements with the NaI detector, which provides integrated estimates of ¹³⁷Cs within the field of view (3.1 m²) of each measurement. There was no dependency of ¹³⁷Cs on pH, clay content and carbon content, but a close relationship was determined between measured ¹³⁷Cs activities and soil moisture. Thus, in-situ data must be corrected for soil moisture. Close correlation (R² = 0.86, p < 0.0001) was found for ¹³⁷Cs activities (in Bq kg⁻¹) estimated with in-situ (NaI detector) and laboratory (GeLi detector) methods. We thus concluded that the NaI detector system is a suitable tool for in-situ measurements in alpine environments. This paper describes the calibration of the NaI detector system for field application under elevated ¹³⁷Cs activities originating from Chernobyl fallout.     

Distribution of uranium isotopes in surface water of the Llobregat river basin (Northeast Spain)

A study is presented on the distribution of ²³⁴U, ²³⁸U, ²³⁵U isotopes in surface water of the Llobregat river basin (Northeast Spain), from 2001 to 2006. Sixty-six superficial water samples were collected at 16 points distributed throughout the Llobregat river basin. Uranium isotopes were measured by alpha spectrometry (PIPS detectors). The test procedure was validated according to the quality requirements of the ISO17025 standard. The activity concentration for the total dissolved uranium ranges from 20 to 261 mBq L⁻¹. The highest concentrations of uranium were detected in an area with formations of sedimentary rock, limestone and lignite. A high degree of radioactive disequilibrium was noted among the uranium isotopes. The ²³⁴U/²³⁸U activity ratio varied between 1.1 and 1.9 and the waters with the lowest uranium activity registered the highest level of ²³⁴U/²³⁸U activity ratio. Correlations between uranium activity in the tested water and chemical and physical characteristics of the aquifer were found.     

Determination of radionuclide levels in rainwater using ion exchange resin and γ-spectrometry

The evaluation of radioactivity accidentally released into the atmosphere involves determining the radioactivity levels of rainwater samples. Rainwater scavenges atmospheric airborne radioactivity in such a way that surface contamination can be deduced from rainfall rate and rainwater radioactivity content. For this purpose, rainwater is usually collected in large surface collectors and then measured by γ-spectrometry after such treatments as evaporation or iron hydroxide precipitation. We found that collectors can be adapted to accept large surface (diameter 47 mm) cartridges containing a strongly acidic resin (Dowex AG 88) which is able to quantitatively extract radioactivity from rainwater, even during heavy rainfall. The resin can then be measured by γ-spectrometry. The detection limit is 0.1 Bq per sample of resin (80 g) for ¹³⁷Cs. Natural ⁷Be and ²¹⁰Pb can also be measured and the activity ratio of both radionuclides is comparable with those obtained through iron hydroxide precipitation and air filter measurements. Occasionally ²²Na has also been measured above the detection limit. A comparison between the evaporation method and the resin method demonstrated that 2/3 of ⁷Be can be lost during the evaporation process. The resin method is simple and highly efficient at extracting radioactivity. Because of these great advantages, we anticipate it could replace former rainwater determination methods. Moreover, it does not necessitate the transportation of large rainwater volumes to the laboratory.     

Evaluation of Monte Carlo-based calibrations of HPGe detectors for in situ gamma-ray spectrometry

The aim of this work was to evaluate the use of Monte Carlo-based calibrations for in situ gamma-ray spectrometry. We have performed in situ measurements at five different sites in Sweden using HPGe detectors to determine ground deposition activity levels of ¹³⁷Cs from the 1986 Chernobyl accident. Monte Carlo-calculated efficiency calibration factors were compared with corresponding values calculated using a more traditional semi-empirical method. In addition, results for the activity ground deposition were also compared with activity densities found in soil samples. In order to facilitate meaningful comparisons between the different types of results, the combined standard uncertainty of in situ measurements was assessed for both calibration methods. Good agreement, both between the two calibration methods, and between in situ measurements and soil samples, was found at all five sites. Uncertainties in in situ measurements for the given measurement conditions, about 20 years after the fallout occurred, were found to be in the range 15–20% (with a coverage factor k = 1, i.e. with a confidence interval of about 68%).     

Non-agglutinating cholera-like Vibrios in sewage,surface water and sea water

Routine bacteriological analysis of sewage work effluents and surface waters has not revealed evidence of Vibrio cholerae or Vibrio El Tor, whereas, non-agglutinating cholera vibrios of Heiberg's groups I and II [so-called non-agglutinating strains (NAG)] have been detected quite frequently. This frequency of NAG presence is approximately equivalent to the presence of Salmonella. Depending on local conditions, quantitative studies of equal amounts of sewage resulted in a ratio of about 1 NAG/10²Salmonella/10⁷E. coli.When it became known that NAG vibrios were capable of producing a clinical appearance in man that resembled cholera by its symptoms and severeness, NAG vibrios raised epidemiological interest. Unlike Salmonella, the nutrient requirements of NAG vibrios are moderate. The decisive factors for their persistence in the environmental are attributed to a certain chloride content in the water and an elevated pH value. Both factors are preferably present in sea water. Over a period of 3 yr, samples of water from the Baltic Sea (Lübecker Bucht) were regularly examined for the presence of NAG vibrios. During this period, there have been a number of positive findings in a sample of 100 ml water while identical samples were always Salmonella-negative.     

Measuring the radium quartet (Ra, Ra, Ra, Ra) in seawater samples using gamma spectrometry

Radium isotopes are widely used in marine studies (eg. to trace water masses, to quantify mixing processes or to study submarine groundwater discharge). While ²²⁸Ra and ²²⁶Ra are usually measured using gamma spectrometry, short-lived Ra isotopes (²²⁴Ra and ²²³Ra) are usually measured using a Radium Delayed Coincidence Counter (RaDeCC). Here we show that the four radium isotopes can be analyzed using gamma spectrometry. We report ²²⁶Ra, ²²⁸Ra, ²²⁴Ra, ²²³Ra activities measured using low-background gamma spectrometry in standard samples, in water samples collected in the vicinity of our laboratory (La Palme and Vaccarès lagoons, France) but also in seawater samples collected in the plume of the Amazon river, off French Guyana (AMANDES project). The ²²³Ra and ²²⁴Ra activities determined in these samples using gamma spectrometry were compared to the activities determined using RaDeCC. Activities determined using the two techniques are in good agreement. Uncertainties associated with the ²²⁴Ra activities are similar for the two techniques. RaDeCC is more sensitive for the detection of low ²²³Ra activities. Gamma spectrometry thus constitutes an alternate method for the determination of short-lived Ra isotopes.     

Radon measurements by nuclear track detectors in secondary schools in Oke-Ogun region, Nigeria

Radon measurements were performed in secondary schools in the Oke-Ogun area, South-west, Nigeria, by solid state nuclear track detectors (SSNTDs). About seventy CR-39 detectors were distributed in 35 high schools of the Oke-Ogun area. The CR-39 detectors were exposed in the schools for 3 months and then etched in NaOH 6 N solution at 90 °C for 3 h. The tracks were counted manually at the microscope and the radon concentration was determined at the Radioactivity Laboratory, Department of Physics, University of Trieste, Trieste, Italy. The overall average radon concentration in the surveyed area was 45 ± 27 Bq m⁻³. The results indicate no radiological health hazard. The research also focused on parameters affecting radon concentrations such as the age of the building in relation to building materials and floor number of the classrooms. The results show that radon concentrations in ground floors are higher than in upper floors.     

Thermal neutron fluence from ultra low-level γ-ray spectrometry of spoons activated during the JCO criticality accident at Tokai-mura in 1999

During the JCO-accident in Tokai-mura in 1999, the surrounding village was irradiated by an uncontrolled neutron flux. At some locations in that village, the thermal neutron flux was determined retrospectively by measurement of the very low activity of ⁵¹Cr and ⁶⁰Co in stainless-steel spoons using γ-ray spectrometry in underground laboratories. Activities determined in the HADES underground facility are presented here, together with calibrations performed using a well-defined thermal neutron flux to directly estimate the fluence of thermal neutrons independent of most assumptions. The results show measurable ⁵¹Cr in three samples and ⁶⁰Co in four samples taken from locations at distances of up to 430 m from the accident location despite the elapse of 4 half-lives of ⁵¹Cr before measurement. Effects of air transport of the samples were considered and shown to be negligible.     

Speciation patterns of actinides in natural waters: a laboratory investigation

The results of laboratory investigations of actinide speciation in ground waters of varying compositions are summarized, re-evaluated and further interpreted, with the inclusion of additional data. Actinide speciation (solubility, oxidation state distributions) in these water samples exhibits great variability at 10⁻¹⁰ to 10⁻⁸ M total actinide concentrations. Americium solubility appears to be controlled by the formation of radiocolloids. neptunium is predictably oxidized and soluble in these water samples, with only a few exceptions. Plutonium exhibits widely varying oxidation state distributions—and hence solubility— despite the presence of 6 mg liter⁻¹ dissolved oxygen in all experiments. Plutonium solubility is enhanced by carbonate and fluoride but is diminished by sulfate in reducing waters. In general, these results are compatible with the limited information available for actinide speciation from previous in-situ investigations but they emphasize the paucity of accurate thermodynamic data to describe these systems.     

Cs, Pu concentrations and the Pu/Pu atom ratio in a sediment core from the sub-aqueous delta of Yangtze River estuary

A sediment core collected from the sub-aqueous delta of the Yangtze River estuary was subjected to analyses of ¹³⁷Cs and plutonium (Pu) isotopes. The ¹³⁷Cs was measured using γ-spectrometry at the laboratories at the Nanjing University and Pu isotopes were determined with Accelerator Mass Spectrometry (AMS), measurements made at the Australian National University. The results show considerable structure in the depth concentration profiles of the ¹³⁷Cs and ^239+240Pu. The shape of the vertical ¹³⁷Cs distribution in the sediment core was similar to that of the Pu. The maximum ¹³⁷Cs and ^239+240Pu concentrations were 16.21 ± 0.95 mBq/g and 0.716 ± 0.030 mBq/g, respectively, and appear at same depth. The average ²⁴⁰Pu/²³⁹Pu atom ratio was 0.238 ± 0.007 in the sediment core, slightly higher than the average global fallout value. The changes in the ²⁴⁰Pu/²³⁹Pu atom ratios in the sediment core indicate the presence of at least two different Pu sources, i.e., global fallout and another source, most likely close-in fallout from the Pacific Proving Grounds (PPG) in the Marshall Islands, and suggest the possibility that Pu isotopes are useful as a geochronological tool for coastal sediment studies. The ¹³⁷Cs and ^239+240Pu inventories were estimated to be 7100 ± 1200 Bq/m² and 407 ± 27 Bq/m², respectively. Approximately 40% of the ^239+240Pu inventory originated from the PPG close-in fallout and about 50% has derived from land-origin global fallout transported to the estuary by the river. This study confirms that AMS is a useful tool to measure ²⁴⁰Pu/²³⁹Pu atom ratio and can provide valuable information on sedimentary processes in the coastal environment.     

Uranium and thorium in soils,mineral sands,water and food samples in a tin mining area in Nigeria with elevated activity

The activity concentrations of uranium and thorium have been determined in soils and mineral sands from the Nigerian tin mining area of Bisichi, located in the Jos Plateau, and from two control areas in Nigeria (Jos City and Akure) using high-purity germanium detectors (HPGe). High resolution sector field inductively coupled plasma mass spectroscopy (HR-SF-ICP-MS) was used to determine uranium and thorium in liquids and foodstuffs consumed locally in the mining area. The activities of uranium and thorium measured in the soils and mineral sands from Bisichi ranged from 8.7 kBq kg⁻¹ to 51 kBq kg⁻¹ for ²³⁸U and from 16.8 kBq kg⁻¹ to 98 kBq kg⁻¹ for ²³²Th, respectively. These values were significantly higher than those in the control areas of Jos City and Akure and than the reference values reported in the literature. They even exceeded the concentrations reported for areas of high natural radioactive background. Radionuclide concentrations in samples of the local foodstuffs and in water samples collected in Bisichi were found to be higher than UNSCEAR reference values. The results reveal the pollution potential of the mining activities on the surrounding areas.     

Study of total organic halogen as a means to detect groundwater contamination

Total organic halogen (TOX) was evaluated as a means to detect contamination of groundwater by halogenated organics. Groundwater samples from monitoring wells at 10 Canadian landfill sites were analyzed for carbon adsorbable TOX, total organic carbon and volatile organics. Low concentrations of TOX (range, ND-44; median 8 μg Cl L^?1) were found at nine sites, and elevated TOX levels (?2072 μg Cl L^?1) at the tenth site. This latter site was studied in greater detail, and TOX and GC-MS analyses were carried out for volatile, base neutral, and acid extractable fractions of the water in six monitoring wells at this site. The TOX and GC-MS techniques were found to provide complementary information. GC-MS analysis detected high concentrations of 1,2-dichloroethylene, trichloroethylene, toluene, and ethylbenzene in some of the wells. TOX measurements, however, indicated the presence of halogenated contaminants in the base-neutral and acid extractable fractions, which had not been detected by GC-MS.     

Environmental radioactivity measurements in Switzerland

The survey of the environmental radioactivity in Switzerland is the responsibility of the Swiss Federal Radioactivity Surveillance Commission (KUeR).All laboratories specialized in environmental radioactivity measurements in Switzerland take part in the KUeR-sampling and measurement program. This program includes measurements of air, water, soil, grass, important food sources as well as the body radioactivity of human beings.This program and the various measuring methods are based on the experience on fall-out measurements of the KUeR and of various international bodies.Special environmental sampling and measurement programs are implemented in the vicinity of the operating Nuclear Power Stations (NPS) and those under construction. To confirm compliance with the licensing requirements the various activities include all measurements to assess any radiological consequences of NPS operation. Such requirements are drawn up for each power-station by the Nuclear Safety Division of the Swiss Federal Office of Energy (ASK) and the KUeR.They include various measurements and techniques starting from the release-point, to dose estimation from external radiation (plum exposure), dose estimation from internal radiation (ecological pathway) and in some cases whole body counting of persons.In our laboratories and national and international round-robin measurements programs we think it will be useful to include standards developed under the auspices of the ICRM.     

Chemical and microbiological examination of well and Nile water

The chemical composition and microbiological contamination of well water and Nile River water used for drinking were investigated in localities around Khartoum, Sudan, to present baseline data. The chemical analyses results obtained indicated that public health hazards due to pH, Ca⁺⁺, CO₃^??, HCO₃^?, and NO₃^? are unlikely in all the samples studied, while Na⁺ and Cl^? ions concentrations in well water warrant some attention. Contamination from organic matter and suspended material is also negligible. Microbial contamination with coliform and fecal coliform is high in surface wells and in the Nile River, but negligible in deep bores, tap water, and mineral water. The logarithm of the colony count ranges from zero for mineral water to 6.8 for water from the White Nile. In addition to drawing further attention to the well water and Nile water used for drinking by a wide sector of the population, the microbial count data for water from the Nile disagreed with the generally held belief that the Nile, being one of the largest rivers of the world, carries no detectable fecal contamination. Our data also did not support the belief that the White Nile is more contaminated than the Blue Nile.     

In-field radon measurement in water: a novel approach

This paper presents a novel approach of measuring radon in-water in the field by inserting a MEDUSA gamma-ray detector into a 210 L or 1000 L container. The experimental measurements include investigating the effect of ambient background gamma-rays on in-field radon measurement, calibrating the detector efficiency using several amounts of KCl salt dissolved in tap water, and measuring radon in borehole water. The results showed that there is fairly good agreement between the field and laboratory measurements of radon in water, based on measurements with Marinelli beakers on a HPGe detector. The MDA of the method is 0.5 Bq L⁻¹ radon in-water.