Airborne concentrations and chemical considerations of radioactive ruthenium from an undeclared major nuclear release in 2017.

In October 2017, most European countries reported unique atmospheric detections of aerosol-bound radioruthenium (106Ru). The range of concentrations varied from some tenths of µBq·m-3 to more than 150 mBq·m-3 The widespread detection at such considerable (yet innocuous) levels suggested a considerable release. To compare activity reports of airborne 106Ru with different sampling periods, concentrations were reconstructed based on the most probable plume presence duration at each location. Based on airborne concentration spreading and chemical considerations, it is possible to assume that the release occurred in the Southern Urals region (Russian Federation). The 106Ru age was estimated to be about 2 years. It exhibited highly soluble and less soluble fractions in aqueous media, high radiopurity (lack of concomitant radionuclides), and volatility between 700 and 1,000 °C, thus suggesting a release at an advanced stage in the reprocessing of nuclear fuel. The amount and isotopic characteristics of the radioruthenium release may indicate a context with the production of a large 144Ce source for a neutrino experiment.

Evidence against solar influence on nuclear decay constants.

The hypothesis that proximity to the Sun causes variation of decay constants at permille level has been tested and disproved. Repeated activity measurements of mono-radionuclide sources were performed over periods from 200 days up to four decades at 14 laboratories across the globe. Residuals from the exponential nuclear decay curves were inspected for annual oscillations. Systematic deviations from a purely exponential decay curve differ from one data set to another and are attributable to instabilities in the instrumentation and measurement conditions. The most stable activity measurements of alpha, beta-minus, electron capture, and beta-plus decaying sources set an upper limit of 0.0006% to 0.008% to the amplitude of annual oscillations in the decay rate. Oscillations in phase with Earth's orbital distance to the Sun could not be observed within a 10-6 to 10-5 range of precision. There are also no apparent modulations over periods of weeks or months. Consequently, there is no indication of a natural impediment against sub-permille accuracy in half-life determinations, renormalisation of activity to a distant reference date, application of nuclear dating for archaeology, geo- and cosmochronology, nor in establishing the SI unit becquerel and seeking international equivalence of activity standards.

Validation of efficiency transfer for high-density materials in HPGe spectrometry.

Recycling and conventional reuse of lead materials and structures originating from controlled areas in nuclear facilities rely on historical knowledge and well selected characterization procedures. At the SCK•CEN, one of these procedures involves performing high-resolution gamma-ray spectrometry measurements on several cylindrical shaped test samples (50 mm diameter and approximately 5 mm thickness), obtained during the lead melting campaigns. The high density (11.3 g/cm³) of these samples is a challenge for radionuclide analysis by gamma-ray spectrometry since no such calibration sources nor reference materials are available. We used the efficiency transfer procedure, relying on regular standard sources available in our laboratory, to set up calibrations for this specific counting geometry. The method proves to be fit for purpose.

Investigation of a new approach for 36Cl determination in solid samples using plastic scintillators.

This work reports a new approach for the determination of 36Cl in radioactive waste samples from nuclear decommissioning, wherein novel plastic scintillator (PS) materials were used for the concentration of 36Cl prior to the detection with scintillation counting. Different plastic scintillator (PS) materials were tested for their selective absorption and detection of 36Cl activity in solid samples. PS microspheres (PSm), cross-linked PSm (CPSm) and PS resin have been investigated. PS resin was identified as the most suitable material for 36Cl analysis. Pyrolysis and subsequent trapping of the volatile elements in a bubbler was used. The trapping solution was finally loaded onto a cartridge of the PS resin. Scintillation counting and ion chromatography were used to determine the activity concentration and the chemical recovery, respectively.

A comparison of different approaches for the analysis of 36Cl in graphite samples.

This study compares different approaches for the quantification of the massic activity of 36Cl in graphite samples. All approaches consisted of a combustion step in combination with a trapping solution to collect the volatile elements. Two different resins were used to separate 36Cl from the matrix (CL resin and PS resin). Liquid scintillation counting (LSC), scintillation counting (SC) and tandem inductively coupled plasma mass spectrometry (ICP-MS/MS) were used to quantify 36Cl activity. The chemical yield in all approaches was determined by means of ion chromatography (IC). In addition, the methods were applied to a real activated graphite sample.

A Monte Carlo method for calculation of the characteristic limits decision threshold and detection limit in low-level radioactivity measurements.

In this study, calculation of decision threshold and detection limit expressed in counts for low-level radioactivity measurements were evaluated and compared to a Monte Carlo method for the case of paired Poisson-distributed observations, i.e. for discrete variables. The calculated characteristic limits obtained from Monte Carlo calculations were compared with analytical expressions given in literature. The results in this study show that the equations given by Currie are in good agreement with the results from the Monte Carlo calculations simulating nuclear counting applications with a low number of observed counts. An exception is observed for a background corresponding to zero counts. This study also shows that at a low number of counts, the specific boundary conditions of the interval that represents counts corresponding to the presence of the analyte (>or ≥), have an impact on the false positives and negatives rates as defined by the parameters α and ß.

Calculation of decision threshold and detection limit in radiometric measurements using a Monte Carlo Method.

Calculation of the decision threshold and detection limit of a measurement, or measurement method, are crucial in order to decide if an analyte is present or not and with what confidence it can be quantified. That decision is important in view of possible actions if something would be detected. In this work, a method for calculating these limits using a Monte Carlo method is presented. In the Monte Carlo method any a priori distribution (e.g. normal distribution, rectangular distribution, triangular distribution) of an input quantity can be selected. Differences between the Monte Carlo calculated characteristic limits and the ones calculated according to ISO 11929:2010 is presented. Moreover, suggestions how to calculate the detection limit when it can not be calculated according to the ISO 11929:2010 are given.

Interception of radionuclides by planophile crops: A simple semi-empirical modelling approach in case of nuclear accident fallout.

Shortly after an atmospheric release, the interception of radionuclides by crop canopies represents the main uptake pathway leading to food chain contamination. The food chain models currently used in European emergency decision support systems require a large number of input parameters, which inevitably leads to high model complexity. In this study, we have established a new relationship for wet deposited radionuclides to simplify the current modelling approaches. This relationship is based on the hypothesis that the stage of plant development is the key factor governing the interception of radionuclides by crops having horizontally oriented leaves (planophile crops). The interception fraction (f) and the leaf area index normalized (fLAI) and mass normalized (fB) interception fractions were assessed for spinach (Spinacia oleracea) and radish (Raphanus sativus) at different stages of plant development and for different contamination treatments and plant densities. A database of 191 f values for Cs-137 and Th-229 was built and complemented with existing literature covering various radionuclides and crops with similar canopy structure. The overall f increased with the plant growth, while the reverse was observed for fB. The fLAI significantly decreased by doubling the contaminated rainfall deposited. Fitting a multiple linear regression to predict the f value as a function of the standing biomass (B), and the radionuclide form (anion and cation) led to a better estimation of the interception (R2 = 81%) than the ECOSYS-87 model (R2 = 35%). Hence, the simplified modelling approach here proposed seems to be a suitable risk assessment tool as fewer parameters will minimize the model complexity and facilitate the decision-making procedures in case of emergencies, when countermeasures need to be identified and implemented promptly.

On the sequential separation and quantification of 237Np, 241Am, thorium, plutonium, and uranium isotopes in environmental and urine samples.

The implementation of the one-pass-through separation technique using two stacked chromatography columns of TEVA - TRU resins for the separation of 237Np, 241Am, thorium, plutonium and uranium from environmental and urine samples was investigated. The sequential separation technique proved to be successful and gave similar results to those obtained when using individual separations. The analysis time was considerably improved. The amount of chemical waste was also reduced by 50% and the use of HClO4 was avoided. The technique of ICP-MS was also investigated as a complementary technique to alpha-spectrometry.

Is decay constant?

Some authors have raised doubt about the invariability of decay constants, which would invalidate the exponential-decay law and the foundation on which the common measurement system for radioactivity is based. Claims were made about a new interaction - the fifth force - by which neutrinos could affect decay constants, thus predicting changes in decay rates in correlation with the variations of the solar neutrino flux. Their argument is based on the observation of permille-sized annual modulations in particular decay rate measurements, as well as transient oscillations at frequencies near 11 year-1 and 12.7 year-1 which they speculatively associate with dynamics of the solar interior. In this work, 12 data sets of precise long-term decay rate measurements have been investigated for the presence of systematic modulations at frequencies between 0.08 and 20 year-1. Besides small annual effects, no common oscillations could be observed among α, ß-, ß+ or EC decaying nuclides. The amplitudes of fitted oscillations to residuals from exponential decay do not exceed 3 times their standard uncertainty, which varies from 0.00023 % to 0.023 %. This contradicts the assertion that 'neutrino-induced' beta decay provides information about the deep solar interior.

Systematic influences on the areas of peaks in gamma-ray spectra that have a large statistical uncertainty.

A method is presented for calculating the expected number of counts in peaks that have a large relative peak-area uncertainty and appear in measured gamma-ray spectra. The method was applied to calculations of the correction factors for peaks occurring in the spectra of radon daughters. It was shown that the factors used for correcting the calculated peak areas to their expected values decrease with an increasing relative peak-area uncertainty. The accuracy of taking the systematic influence inducing the correction factors into account is given by the dispersion of the correction factors corresponding to specific peaks. It was shown that the highest accuracy is obtained in the peak analyses with the GammaVision and Gamma-W software.

Characterization of the natural radioactivity of the first deep geothermal doublet in Flanders, Belgium.

Deep geothermal energy is a local energy resource that is based on the heat generated by the Earth. As the heat is continuously regenerated, geothermal exploitation can be considered as a renewable and, depending on the techniques used, a sustainable energy production system. In September 2015, the Flemish Institute for Technological Research (VITO) started drilling an exploration well targeting a hot water reservoir at a depth of about 3km on the Balmatt site near Mol. Geothermal hot water contains naturally occurring gases, chemicals and radionuclides at variable concentrations. The actual concentrations and potentially related hazards strongly depend on local geological and hydrogeological conditions. This paper summarizes the radiological characterization of several rock samples obtained from different depths during the drilling, the formation water, the salt and the sediment fraction. The results of our analyses show low values for the activity concentration for uranium and thorium in the formation water and in the precipitate/sediment fraction. Also, the activity concentrations of 210Pb and 210Po are low in these samples and the activity concentration of 226Ra is dominant. From the analysis of the rock samples, it was found that the layer above the reservoir has a higher uranium and thorium concentration than the layer of the reservoir, which on the other hand contains more radium than the layer above it.

Assessing sample attenuation parameters for use in low-energy efficiency transfer in gamma-ray spectrometry.

We present a numerical fitting method for transmission data that outputs an equivalent sample composition. This output is used as input to a generalised efficiency transfer model based on the EFFTRAN software integrated in a LIMS. The procedural concept allows choosing between efficiency transfer with a predefined sample composition or with an experimentally determined composition based on a transmission measurement. The method can be used for simultaneous quantification of low-energy gamma emitters like (210)Pb, (241)Am, (234)Th in typical environmental samples.

Determination of 210Pb, 210Po, 226Ra, 228Ra and uranium isotopes in drinking water in order to comply with the requirements of the EU 'Drinking Water Directive.

The European Union published in 2013 a new Drinking Water Directive with stricter requirements for measuring natural radioactivity. In order to adhere to this, a method for sequential separation of 210Pb, 210Po, 238U and 234U in drinking water was applied using UTEVA® and Sr resins. Polonium-210, 238U and 234U were quantified using alpha-particle spectrometry and 210Pb using liquid scintillation counting. Radium-226 and 228Ra were determined using 3M Empore Radium RAD Disks, and their quantification was done using a Quantulus™ 1220 liquid scintillation counter.

A computerised system for the identification of lactic acid bacteria.

A generic computerised system for the identification of bacteria was developed. The system is equipped with a key to the identification of lactic acid bacteria. The identification is carried out in two steps. The first step distinguishes groups of bacteria by following a decision tree with general identification tests. The second step in the identification is the distinction of species within a group on the basis of biochemical fermentation patterns. During grouping, probabilities for test failure are used. These probabilities can be used for assessing the quality of a given test answer. The probabilities are also used to select the most probable test answer in cases where the test result is inconclusive. The probabilities of test failure were determined by a group of experts and a group of potential users of the identification system. During species identification, similarity indices are calculated for all bacteria in a group. The described identification system has the ability to "learn" from different sessions in the species identification step, improving both identification speed and accuracy. Because of the versatile way in which the system is set up, it can very easily be expanded with identification keys to other organisms.

[Follow-up of patients with colorectal cancer resected for cure in the Herault area. A medico-economical study]. / Surveillance des malades opérés à visée curative d'un cancer colorectal dans le département de l'Hérault.

UNLABELLED: Optimal modalities of surveillance of colorectal cancers (CRC) resected for cure have not been determined so far and the overall improvement of 5-year survival related to surveillance has not been demonstrated. AIM OF THE STUDY: To retrospectively evaluate modalities, results and costs of follow-up of patients during the 5 years following the resection for cure of CRC. METHODS: We studied medical and economical data from records of 256 patients registered in the cancer registry of the Herault area who underwent a potentially curative resection of CRC in 1992. We analyzed comparatively modalities of follow-up in patients who were followed according to recommendations from the 1998 French consensus conference (standard follow-up) and in those who had a simplified follow-up. We evaluated cumulative costs of follow-up. RESULTS: Nine patients died in the postoperative period. Recurrence rate was 27% (69 patients). Sixty-nine patients had a standard follow-up (30% of the 231 classified patients) and 162 patients (70%) had a simplified follow-up. The specific survival rate (taking into account only death related to CRC) 5 years after resection for cure was 75%. The 5-year specific survival rate after diagnosis of recurrence was 12% in the patients with recurrent disease within the 5 years after initial therapy. The 5-year survival rate after standard and simplified follow-up were 85% and 79%, respectively (P=0.25). Total cost of follow-up of the 256 patients was 1 085 507 French francs (FF). Mean follow-up cost per patient was 5 527 FF. Cost of the examinations not recommended by the consensus conference represented 30% of the expenses. Individual total cost of the follow-up of patients alive 5 years after the diagnosis of the recurrence was 120 356 FF. CONCLUSION: In Herault area, clinicians carried out in 70% of the patients a simplified follow-up and in 30% of the cases a reinforced follow-up in comparison with French recommendations. Survival rates were not significantly different between the 2 groups.

The in vivo assessment of thorium body burden by gamma ray sepctrometry.

Thorium is used in many different industrial technologies and is widely found in nature. Internal contamination with thorium is considered as highly hazardous because of its radiological and chemical toxicities, which depend on the chemical form in which thorium appears. The assessment of the thorium body burden is then of primary importance in detecting the risks of personal contamination, and for appropriate counteractions when contamination is detected. The in vivo assessment of the thorium lung burden is commonly achieved by gamma ray spectrometry of its progeny. Three methods for the assessment of thorium in the lungs are compared. In the first method, the radionuclide examined is 208Tl, measured with a Nal(TI) detector. This simple method can be affected by systematic errors due to 220Rn exhalation and because of the assumption of equilibrium between 232Th and 228Th. The second method, based on the measurement of the gamma rays emitted by 228Ac, requires the use of high-resolution gamma spectrometry (HPGe detectors). The accuracy of the thorium quantification is better with this technique. The third method is based on the measurement of exhaled 220Rn.

[Experience with peripheral vascular injures from 1965-1980]. / Ervaring met perifere vasculaire traumata van 1965-1980.

The authors analyse a series of 45 vascular trauma treated during the period 1965-1980. It is very important to make a diagnosis as soon as possible and to limit the interval accident-operation. In 40% of our cases we had to operate rather late. Most of those cases were secondary transfers of other hospitals. Arteriography should be performed if there is any doubt. Now we always perform an angiogram during the operation. If there is any associated orthopedic injury, this is handled first, if possible by external fixation. A fasciotomy can be of value to save a limb. Any venous injury should be repaired also.

A dedicated LIMS for routine gamma-ray spectrometry.

We developed a Microsoft(®) Access-based LIMS (Laboratory Information and Management Systems), γ-LIMS, for the management of our gamma-spectrometry laboratory, in which thousands of routine, but high-quality analyses are performed each year. This paper explains the main features of the γ-LIMS and puts special attention on the interfacing methods and solutions for using the Genie™2000 spectrometry software in conjunction with the EFFTRAN package, which serves for efficiency transfer calculations, coincidence summing corrections and a procedure for uncertainty estimation.

Efficiency calibration of BEGe and extended range detectors.

Any approach to efficiency calibration of HPGe detectors sensitive to low-energy gamma-rays and X-rays has to deal with true coincidence summing. We developed a method based on the integration of the EFFTRAN code into the commercial Genie2K™ gamma-ray spectrometry software. EFFTRAN's role is to compute true coincidence summing corrections and to obtain satisfactory results for detectors sensitive to X-rays. EFFTRAN had to be upgraded to include a full simulation of the emission of X-rays. In this manner, efficiency calibrations were successfully set up for BeGe and XtRa detectors.