Direct and precise determination of environmental radionuclides in solid materials using a modified Marinelli beaker and a HPGe detector

A simple but precise detection method was studied for the determination of natural radionuclides using a conventional HPGe detector. A new aluminium beaker instead of a plastic Marinelli beaker was constructed and examined to reach radioactive equilibrium conditions between radon and its daughter elements without the escape of gaseous radon. Using this beaker fifteen natural radionuclides from three natural decay series could be determined by direct γ-ray measurement and sixteen radionuclides could be determined indirectly after radioactive equilibrium had been reached. Analytical results from ground water were compared with those from conventional α spectroscopy and the results agreed well within 12% difference. Nitrogen gas purge was used to replace the surrounding air of the detector to obtain a stable background and reducing the interference of radon daughter nuclides in the atmosphere. The use of nitrogen purging and the aluminium Marinelli beaker results in an approximately tenfold increase of sensitivity and a decrease of the detection limit of ²²⁶Ra to about 0.74 Bq kg^–1 in soil samples. Received: 12 October 2000 / Revised: 12 December 2000 / Accepted: 13 December 2000     

Measurement of radioactive samples in Marinelli beakers by gamma-ray spectrometry

Radioactivity measurement of environmental samples is frequently assayed by gamma-ray spectrometry using Marinelli beakers. In this work, self-absorption and coincidence summing effects arising in activity measurements for Marinelli beaker geometry have been studied with a Ge detector. Three types of Marinelli beakers which have capacities of 450 mL, 1 L, and 2 L were developed. Self-attenuation effects for density variation of radioactive samples in each type of the Marinelli beakers were measured as a function of gamma-ray energy, and also the results were compared with calculated values by mathematical model. Meanwhile, the coincidence summing effects of¹²⁵Sb and¹⁵⁴Eu nuclides were obtained from the determination of the full-energy peak and total efficiencies for a Ge detector.     

Estimation of true coincidence corrections for voluminous sources

To analyze a voluminous radioactive source with the highest possible sensitivity, it is necessary to use both a high efficiency detector and an optimal measurement geometry. The optimal geometry implies positioning the source as close to the detector as possible. It also implies selection of the shape of the source in order to reach the highest efficiency possible (e.g., Marinelli beaker). Under such conditions of measurements, true coincidences may cause systematic errors that can reach levels of more than ten percent for some radionuclides. A method for estimation of the effect of these coincidences was developed. It is based on direct computation of the effect by means of integration of a function which involves the experimentally obtained detection efficiency for the place around the detector. It was found that for the tested detector with a relative efficiency of 15%, the so-called intrinsic peak-to-total calibration may be used in the course of such an integration: It has been shown that theP/T-ratio for the given energy in the working space around the detector may be considered a constant value. Some results from a peak-to-total calibration study in the presence of scattering material are also given.The main part of the material has been presented at the Third International Meeting Nuclear Methods for Protection of the Environment, May 1995, Dubna, Russia.     

A method for self-attenuation and sample-height correction for counting efficiency of HPGe using Marinelli beaker geometry

A procedure for self-attenuation and sample height correction in HPGe gamma spectrometry efficiency has been presented. An MCNP model of an HPGe detector was used to calculate the full energy peak efficiency (FEPE) for a group of different samples with different heights in Marinelli beaker geometry. A proper function has been fitted to the simulation results to obtain the correction function. The function has been used to calculate the FEPE of a spiked soil sample in different sample heights by considering the experimentally known FEPE of another standard solution source. A good agreement between the experiments and calculations have been shown.     

Leaching of uranyl–silica complexes from the host metapelite rock favoring high radon activity of subsoil air: case of Castañar cave (Spain)

Castañar cave is a subterranean site with an outstanding natural environmental radioactivity. The maintaining of high radon activity of cave air and the detection of spatially anomalies of this gas in some cave emplacements, suggests that some natural geochemical processes are involved on the mobilization of radioactivity sources to cave environment, other than a simple exhalation of radon from the host-rock. The host rocks are interlaid dolostone–metapelite beds with radioactive nuclides of the three actinium, thorium and uranium decay series. In situ measurements on the spatial distribution of radioactivity, uranyl group’s luminescence and radon gas concentrations inside cave were main focus of this work to model lixiviation and deposition mechanisms of radioactive elements from the host rock to the karstic system. In addition, collected micro-samples were also analyzed by a multi-approach suite of analytical techniques: inductively coupled plasma mass spectrometry, environmental scanning electron microscopy with an attached X-ray energy dispersive system and spectral cathodoluminescence detector, thermoluminescence, Raman spectroscopy, X-ray diffraction, differential-thermal and thermogravimetry analysis, Alpha-spectrometry and Gamma-spectrometry techniques. The host metapelitic beds contain Zr(Hf)–Th(U)–Ti–P–REE phases such as zircon, xenotime-(Y), monazite-(Ce, La) and poly-metallic mineralization veins of hydrothermal origin. Carbonated host beds and speleothems show frequently chemical elements leaked from the upper host rock masses. The weathering leakage processes are favored by the existence of pyrite and limonite in the dolostone masses. The cave exhibits under UV lamps abundant hydrous silica–uranyl coatings covering carbonated speleothems with radionuclides of ²³⁸U natural decay series. The long-lived radio-nuclides of the radium radioactive decay chain are responsible of the continuous regeneration of radon gas inside cave. The experimental work was focused to identify origin and remobilization processes of radio-nuclides and their latte settlement into the cave environment associated to mineral phases of speleothems and cave deposits.     

Industrial commercial respirator filter as indoor radon monitor

This paper presents a method for measuring indoor radon concentrations using a commercially available air-purifying respirator filter as a component of the radon monitor. The filter used was Survivair’s NIOSH (National Institute for Occupational Health and Safety)-approved 100800 model. The method is based on the diffusion of radon gas into the activated carbon of the filter and the measurement of the radioactive daughters resulting from the radon decay. The photopeaks of the ²¹⁴Bi daughter gamma rays (0.609 MeV) were analyzed with a Hyper-Pure Germanium (HPGe) detector and a multichannel system. A monotonically increasing and very close to linear response relation between the integrated area under the ²¹⁴Bi photopeak and the radon concentration of the activated carbon was found. A well-defined relation held for radon levels ranging from 15 to 4,700 Bq/m³. This procedure results in highly reproducible and reliable measurements of indoor radon levels. Interesting applications include the investigation of radiological accidents involving radon and the retrospective measuring of indoor radon concentrations by analyzing the filters of the respirators worn by personnel working during the relevant period.     

Low gamma counting for measuring NORM/TENORM with a radon reducing system

A detection system for counting low levels of gamma radiation was built by upgrading an existing rectangular chamber made of 18 metric tonne of steel fabricated before World War II. The internal walls, the ceiling, and the floor of the chamber are covered with copper sheets. The new detection system consists of a stainless steel hollow cylinder with variable circular apertures in the cylindrical wall and in the base, to allow introduction of a NaI (Tl) crystal, or alternatively, a HPGe detector in its interior. This counting system is mounted inside the larger chamber, which in turn is located in a subsurface air-conditioned room. The access to the subsurface room is made from a larger entrance room through a tunnel plus a glass anteroom to decrease the air-exchange rate. Both sample and detector are housed inside the stainless steel cylinder. This cylinder is filled with hyper pure nitrogen gas, before counting a sample, to prevent radon coming into contact with the detector surface. As a consequence, the contribution of the ²¹⁴Bi photopeaks to the background gamma spectra is minimized. The reduction of the gamma radiation background near the detector facilitates measurement of naturally occurring radioactive materials (NORM), and/or technologically enhanced NORM (TENORM), which are usually at concentration levels only slightly higher than those typically found in the natural radioactive background.     

Variation of the detection efficiency of a Ge detector with the height of the sample in Marinelli beaker

Several two and three parameter analytical functions were fitted to the measured detection efficiencies () of a Ge detector for a Marinelli beaker filled with samples up to different heights (H). From these, the expression =308E ^–0.82/((H–6.1)²+107), gave the best fit. The measured and calculated efficiencies were compared and for 70 determinations, a relative standard deviation of only 7.6% was obtained.     

A computer program for calculating Ge(Li) detector counting efficiencies for Marinelli beakers

A novel computing method has been developed to calculate the absolute photopeak efficiency of a Ge(Li) detector for Marinelli beakers of different heights and diameters and with variable density. For each point in the cylindrical sample the detection efficiency is calculated taking into account the distance from the detector and gamma-ray attenuation and the efficiency is integrated numerically over the volume of the sample. The detector is approximated as a point detector with an experimentally determined effective interaction depth. It is necessary to measure the absolute efficiency for a point source located on the detector axis and on a line beside the detector parallel to the axis. The computer program calculates the absolute counting efficiency for Marinelli beakers of any geometry and for any density. The measured and calculated values for three different densities give a good (–2.2%) overall agreement.     

High pressure Marinelli for counting low activity compressed gas samples

Quantification of low-activity noble gases in air is typically accomplished through separation of the noble gas from air followed by radiometric assay. This work is aimed at quantification of radioactive noble gas in air without extraction. A high pressure aluminum Marinelli counting vessel was designed and fabricated that can be placed on a coaxial high purity germanium detector for gamma counting. Characterization of the performance of this Marinelli using MCNP modeling, large excesses of activity, and low-activity noble gas in air is discussed. Minimum detectable concentrations achieved during a 24 h count are: 5, 10, 50, and 1 Bq/m³ for ¹³³Xe, ^133mXe, ^131mXe, and ¹³⁵Xe, respectively.     

Factors associated with the variations in environmental gamma-ray spectra in Kashiwazaki Kariwa area

Since October 1983, the Niigata Prefectural Government has been carrying out the continuous measurements of gamma-emitting radionuclides in the environment around the Kashiwazaki Kariwa nuclear power station by environmental radiation monitoring telemetry system. Continuous measurements of gamma-ray spectra have been established since April 1996. As a result, the contribution of various radionuclides has been gradually clarified in the variations of the gamma-ray dose rate. In this paper, the energy spectrum of the incident gamma-ray to NaI(Tl) scintillation detector was obtained by the unfolding method using a response matrix, and the variations of the energy spectrum observed in the precipitation and snow were investigated. The increase in the dose rate in precipitation originated from the increase in the flux density of gamma-ray from ²¹⁴Bi and ²¹⁴Pb, daughter nuclide of ²²²Rn, which fell down with the precipitation. On the other hand, the reduction in the dose rate in the snowy period was confirmed due to the shielding effect of a part of gamma-rays from the natural radioactive nuclides by the snow layer, in coincidence with the decrease of the flux density in ⁴⁰K and ²⁰⁸Tl.     

Bestimmung Kleinster Radium-226 Konzentrationen im Wasser

A sensitive technique is described, which permits, without chemical treatment, detection of radium (²²⁶Ra) in water in concentrations as low as 0.01 pCi·1⁻¹. The determination is based on the emanation of radium daughter radon (²²²Rn) after it has achieved the radioactive equilibrium; it is then counted in a scintillation chamber. This procedure was applied to water samples from public water supplies in Hessia, Germany, for routine measurements. The radium concentration of 205 samples show log-normal distribution with a mean value of 0.11 pCi·1⁻¹ and a geometric standard deviation of 2.6. Significantly higher results, between 0.12 and 14.6 pCi·1⁻¹, were obtained for several samples of commercially available mineral water.

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Herrn Prof. Dr. A. SCHRAUB zum 70. Geburtstag gewidmet.     

Europium removal with a mineral mixtre

Natural mixture containing mostly minerals of iron, sillicon, magnesium, aluminium and calcium was exploited for the decontamination study of europium radionuclides from aqueous radioactive waste solutions. The physicochemical conditions, such as shaking and equilibration time, nature of hydrogen ions, pH, temperature, concentrations of adsorbate and adsorbent were experimentally determined. This study showed quantitative adsorption beyond pH 7 and under optimized conditions, up to 33 g of the adsorbate can be rapidly removed from radioactive effluents using only 1 kg of the mineral mixture (MM). Desorption study of the solidified radioactive waste product reveals no significant loss (< 0.01% month), indicating MM as an effective material for removal of radioactive europium and storing it in solid form over a long period of time.     

Measurement of radon in air by α track method enhancement of detection sensitivity using a lamp

A new α track method is proposed for the measurement of radon (²²²Rn) concentration in environmental levels. This involves collecting radon daughters on the surface of pilot lamp and detecting α-particles emitted from the nuclides (²¹⁸Po and²¹⁴Po) by a detector (LR 115). The detection sensitivity of this method is 6 times greater than that of the conventional α track method.     

Alpha emitters from uranium mining in the environment

Uranium mining and milling activities usually generate an enhancement of radionuclide concentrations in the environment that may cause increased radiological exposure to mankind. For risk assessment and radiological protection of man and environment in these areas, usually, it is needed to implement radiological surveillance of water, soils, agricultural products, aerosols, and mining waste discharges as well. Radionuclides to be monitored in priority are alpha-emitting nuclides of the uranium natural series. Radioactivity analysis of materials from uranium mining areas of Portugal shows departure from secular radioactive equilibrium amongst uranium series radionuclides, thus rendering invalid the assumption of equilibrium and requiring the actual determination of each radionuclide. Radionuclide measurements performed with high resolution alphaspectrometry, as reported herein, produce accurate results on specific radionuclides that are essential in computing radiation doses to critical groups of the population.     

Counting yield calibration of NaI(Tl) detectors for complex geometry samples by use of californium-252

The counting yield for large volume, complex geometry samples such as solutions in Marinelli beakers as counted on a large NaI(Tl) detector can be calibrated using radionuclides activated by neutrons form a²⁵²Cf source. Calibration may be done by using either a known neutron flux facility or by cross calibration of the activated material as a point source vs. sealed gamma-standard sources. The point source of activated material is dissolved after cross calibration to produce the large volume distributed source.     

The importance of radiochemistry for the characterization of NORM and of environments contaminated by NORM

Naturally occuring radioactive materials (NORM) are present in the environment and they can be concentrated by technical activities, particularly those involving natural resources. This article describes radioanalytical problems arising in the accurate determination of natural radionuclides in NORM and in the environment contaminated by NORM. The solution of these problems is of particular importance since the results can be used to estimate the dose to workers and to the population. A special emphasis is given to the reliability of the radiochemical methods and procedures applied for the detection and measurement of alpha or beta emitters by radiometric or non-radiometric techniques.     

Alpha-Particle Dosimetry Using Solid State Nuclear Track Detectors: Application to 222Rn and its daughters

We present a methodology for the determination of the detection efficiency of a solid state nuclear track detector for radon and its short-lived daughters. First, particular attention is paid to the -particles having energies and angles of incidence that lead to observable tracks after an adapted chemical etching. These results are then incorporated in a mathematical model to determine the theoretical radon detection efficiency of a polymeric detector placed in a cylindrical cell. When applied to LR115 and CR39 detectors, the model reveals the influence of the position of the radon daughters inside the cell. Radon daughters tend to link up with natural atmospheric aerosols and then settle on the cell's inside wall. This model allows to determine, among other things, the cell size for which the detector response is independent of the fraction daughters plated out.