Analytical application of Cherenkov radiation

The application of Cherenkov photometry gives a new possibility in isotope dilution analysis for determination of specific activity in a simple way. If the compound of the isotope is coloured or it can be converted into a coloured compound, it is possible to measure the activity and the concentration of the compound in one sample in one series of measurement. Methods were worked out for the determination of³²P specific activity by measuring the³²P efficiency, activity and the phosphorus content of the same sample. It is possible to measure the specific activity in an automatic mode with some modification of the liquid scintillation spectrometer.     

Alpha-beta discrimination liquid scintillation counting for uranium and its daughters

Advances in liquid scintillation counting (LSC) technologies, such as imporved scintillation cocktail formulations and alpha-beta radiation discrimination, make LSC suitable for applications in uranium process chemistry. Ease of use, low cost, and the huge dynamic range of LSC are distinct advantages for analytical support of actinide processing. All uranium isotopes decay primarily with alpha radiation emission. The immediate short-lived daughters of²³⁸U are²³⁴Th and²³⁴Pa. These nuclides are beta emitters having energy bands that overlap the uranium bands in a liquid scintillation spectrum. The resolution of these overlapping bands by alpha-beta radiation discrimination is useful for uranium quantification and purity verification. Protactinium-234 is a high-energy beta emitter that can be further identified and quantified from it's Cherenkov radiation. Energy spectra were collected on the Packard 2500AB liquid scintillator analyzer for uranyl solutions in diisopropylnaphthalene and pseudocumene based scintillator cocktails. Calibration curves were prepared for nitric, hydrochloric, and sulfuric acid media. Base titrations demonstrated the effect of acid quenching on those system. Ion exchange and water soluble polymer extraction studies are readily followed using liquid scintillation methods.     

Adaptation of PTB’s analytical modelling for TDCR–Cherenkov activity measurements at LNHB

Designed for triple to double coincidence ratio measurements based on liquid scintillation, the three-photomultipliers detection system can also be applied for Cherenkov counting using aqueous solutions. For activity determination, a specific modelling of Cherenkov light emission has to be constructed. For that purpose, the analytical modelling first developed at PTB was adapted to account for the physical features of the detection system used at LNHB. The first results are presented in the case of activity measurements of two high-energy β^?-emitters (⁹⁰Y and ⁸⁹Sr). The analytical modelling was also tested for the standardization of ⁶⁸Ge in a solution of ⁶⁸Ge/⁶⁸Ga in equilibrium in the framework of a BIPM international comparison in 2014.     

Evaluation of interferences on measurements of 90Sr/90Y by TDCR Cherenkov counting technique

A study to evaluate conditions affecting the determination of ⁹⁰Sr/⁹⁰Y activities in liquid samples by the triple-to-double coincidence ratio (TDCR) Cherenkov counting technique was conducted. The Cherenkov radiation produced by the ⁹⁰Y beta decay was determined using a commercially available Hidex 300 SL liquid scintillation counter. The interferences of sample geometry, including sample counting vial type and volume composition, and sample colour on the TDCR were investigated. The effects of potentially interfering beta and mixed beta–gamma emitters on the TDCR Cherenkov counting of ⁹⁰Sr/⁹⁰Y activities were also examined. The TDCR values were used to quantify counting efficiencies of ⁹⁰Y under different experimental conditions. The results demonstrated that the Cherenkov counting efficiency of ⁹⁰Y is independent of sample volume and counting vial size. The effect of colour quenching was examined using yellow and brown food-grade dyes. The TDCR correction for colour quenching was found to be effective. An evaluation of counting efficiency of different beta-emitting radionuclides demonstrated that strong gamma emissions can contribute to the Cherenkov counting efficiency. Overall, measured radioactivity values deviated from reference values by ≤7.5 %, which is acceptable for screening applications in emergency situations.     

Determination of 90Sr in radioactive concentrate from Nuclear Power Plant Mochovce

This paper describes the use of molecular recognition technology product AnaLig^®Sr-01 gel from IBC Advanced Technologies, Inc. to effectively and selectively pre-concentrate, separate and recover strontium from evaporator concentrate samples from Nuclear Power Plant Mochovce which belongs to the most difficult matrices to analyze. The method is suitable for analyzing highly contaminated samples of radioactive waste in a relatively short time and with high decontamination factors. Activity of ⁹⁰Sr was measured using Cherenkov counting on TRI CARB 2900 TR liquid scintillation counter.     

Rapid measurement of 241Pu activity at environmental levels using low-level liquid scintillation analysis

A straightforward and rapid method has been developed for the determination of ²⁴¹Pu activities. Pu is chemically separated from the sample, purified and electrodeposited to produce a source for alpha spectrometric determination of ²³⁸Pu and ^239,240Pu. Pu is stripped from the disc with concentrated nitric acid and extracted into tri-octylphosphine oxide (TOPO)/toluene. The organic extract is then mixed directly with commercial liquid scintillation cocktail without any further purification procedures and the sample counted on a Wallac 1220 Quantulus liquid scintillation counter (LSC). ²⁴¹Pu activity is estimated via the ²⁴²Pu yield monitor acquired by alpha spectrometry measurement. Experimental results for the performance testing of a low-level liquid scintillation spectrometer and the data for the evaluation of the method using standard reference materials are presented.     

Detection limit of the cherenkov radiation of204Tl measured with a liquid scintillation counter

The cause of the low detection efficiencies of Cherenkov radiation by the liquid scintillation counter was investigated. The detection limit of the liquid scintillation counter was assumed and the increase of counting rates for the increase of refractive index was calculated from Cherenkov photo yields and -distribution.     

Rapid determination of 90Sr/90Y in water samples by liquid scintillation and Cherenkov counting

Strontium-90 (⁹⁰Sr) is a ubiquitous contaminant at nuclear facilities, found at high concentrations in spent nuclear fuel and radioactive waste. Due to its long half-life and ability to be transported in groundwater, an accurate method for measuring ⁹⁰Sr in water samples is critical to the monitoring program of any nuclear facility. To address this need, a rapid procedure for sequential separation of Sr/Y was developed and tested in groundwater samples collected from an area of riverbed affected by a ⁹⁰Sr groundwater plume. Sixteen samples, plus spike and water blanks, were analyzed. Five different measurements were performed to determine the ⁹⁰Sr and yttrium-90 (⁹⁰Y) activities in the samples: direct triple-to-double-coincidence ratio (TDCR) Cherenkov counting of ⁹⁰Y, liquid scintillation (LS) counting for ⁹⁰Sr following radiochemical separation, LS counting for ⁹⁰Y following radiochemical separation, Cherenkov counting for ⁹⁰Y following radiochemical separation and LS counting of the Sr samples for ⁹⁰Y in-growth. The counting was done using a low-level Hidex 300SL TDCR counter. Each measurement method was compared for accuracy, sensitivity and efficiency. The results following Cherenkov counting and radiochemical separation were in very good agreement with one another.     

Determination of90Sr in environmental and biological materials with combined HDEHP solvent extraction-low liquid scintillation counting technique

Low level⁹⁰Sr in environmental and biological samples is determined using a combined HDEHP solvent extraction-liquid scintillation procedure. Yttrium-90 is selectively extracted from nitric acid solution into 5% di(2-ethylhexyl) phosphoric acid (HDEHP) in toluene, and⁹⁰Y in the organic phase is measured directly using an ultra low level liquid scintillation spectrometer.The working program of the Quantulus counter has been optimized. As the counting efficiency using liquid scintillation counting is high and the stripping and precipitation of Yttrium-90 oxalate is omitted, this procedure is simpler and more timesaving than traditional methods. The chemical recoveries of⁹⁰Y were 85.1% for soil, 75.7% for milk and 65.3% for bone. The detection limit is 8 mBq.     

Absolute liquid scintillation counting of35S and45Ca using a modified integral counting method

The disintegration rates of³⁵S and⁴⁵Ca samples were determined by the modified integral counting method, which extrapolates the integral count rate to the zero detection threshold of a liquid scintillation spectrometer. The agreement between the extrapolated value and the standardized disintegration rate of the sample is very satisfactory.     

The role of Cherenkov and liquid scintilation counting in evaluating the anion-exchange separation of210Pb−210Bi−210Po

Using as eluent a sequence of 3M HCl, 12M HCl, and 8M HNO₃, a mixture of²¹⁰Pb,²¹⁰Bi, and²¹⁰Po may be clearly separated on a column of Dowex 1×2−100 anion exchange resin. A Cherenkov count in H₂O and the variation in count rate with time confirm that the nuclides emerge in the order²¹⁰Pb→²¹⁰Bi→²¹⁰Po. If 12M HCl is replaced by 1.5M H₂SO₄/2.3 M Na₂SO₄, a clean separation also results, but recovery of²¹⁰Po becomes considerably more difficult. All three nuclides are readily detectable by liquid scintillation counting, with the efficiency for²¹⁰Pb in the 60–70% range. The Cherenkov aqueous counting efficiency for²¹⁰Bi is ∼14–15%.     

Improved method for the separation of radioactive strontium from various samples by mixed solvent anion exchange

Procedures for the separation and determination of⁹⁰Sr in liquid samples, with cation and anion exchangers have been described. Strontium, yttrium and other cations bind to the cation exchanger and are eluted from the column by means of nitric acid. Separation of yttrium and strontium from other cations is carried out on columns filled with strong base anion exchangers in nitrate form with alcoholic solutions of nitric acid. This separation method enables the determination of⁹⁰Sr through yttrium on a low-level gas flow α, β-counter, as well as through strontium on a lowlevel liquid scintillation counter by means of Cherenkov counting. Such procedures have been tested by the determination of⁹⁰Sr in water, wine, medium radioactive liquid waste samples, milk and clover samples. For comparison, the determination has also been carried out by the standard method. It has been showed that the developed procedures might produce a high efficiency in strontium separation and a satisfactory accuracy of determination.     

A comparative study using liquid scintillation counting and X-ray spectrometry to determine 55Fe in radioactive wastes

The radionuclide ⁵⁵Fe was determined in samples of radioactive wastes from the water cleanup system of the IEA-R1 nuclear research reactor. In order to validate the results, the ⁵⁵Fe activity concentration was measured in eight waste samples and in six simulated samples containing the most important interfering radionuclides. A simple method was employed to separate and purify ⁵⁵Fe from other radionuclides present in these samples, combining co-precipitation with ammonium hydroxide and purification with anionic ion-exchange resin, which enables ⁵⁵Fe to be quantified either by liquid scintillation counting (LSC) or by X-ray spectrometry using a low-energy germanium spectrometer (LEGe). Both measurement methods were used so that the separation and purification process could be confirmed by comparison of spectra with and without the utilization of anionic ion-exchange resin. Activity and interferences were compared in the results obtained from LSC and LEGe measurement methods.     

Simultaneous biphasic liquid scintillation determination of americium and plutonium

A procedure for the simultaneous determination of²⁴¹Am and²³⁹Pu or²³⁸Pu was carried out in samples such as air filters, sweep-tests, aqueous solutions and urine. The method described here includes a previous treatment of the samples in accordance with the type of matrix in which the actinides are included and a liquid scintillation counting using a two-phase cocktail. The upper detection limit was estimated to be 50 mBq for a 50-minute counting time.     

Measuring alpha and beta activity of filter and swab samples with LSC

Analysis of alpha and beta emitters in aerosol filters and swabs of different materials by liquid scintillation counter is discussed. This method appears suitable for fast determination of activity of radionuclides due to direct alpha and beta separation, measurement in 4π geometry and without sample treatment. The selected group of radionuclides was chosen with respect to military significance, radiotoxicity, and possibility of potential misuse. ⁹⁰Sr and ²³⁹Pu were selected as model radionuclides. Three types of filters were examined, and the attention was also focused on optimizing the type and volume of LSC cocktail. The efficiencies for ²³⁹Pu and ⁹⁰Sr were 90% and 79%, respectively. This method was the most effective for the glass fiber filters measured with the MaxiLight cocktail.     

Development of a Multipurpose Alpha Detection Procedure for Enriched Uranium in Urine

Abstract

An anion exchange-liquid scintillation procedure for detecting enriched uranium alpha emissions in urine is described. Uranium is removed from extraneous elements by anion exchange. The uranium is eluted from the column and extracted into a liquid scintillator before being counted in a photon-electron rejecting alpha liquid scintillation spectrometer. The average recovery was 92 percent at the 0.9 dpm level.     

Liquid scintillation and Cherenkov counting characteristics of109Cd

When¹⁰⁹Cd is placed in a liquid scintillation counter, 146±1 counts are obtained for every 100¹⁰⁹Cd nuclides which undergo decay. Thus, the average efficiency for each of the two steps in the decay process is 73%. In examining the distribution of energy among the windows available, it was noted that the distribution pattern is quite similar to that of¹⁴C. An average Cherenkov counting efficiency, in water, was found to be 0.0258±0.0005%. Both 0.010M K₂Cr₂O₇ and CHCl₃ quench the count rate, particularly in the lower energy channel, where count rates are suppressed by up to a factor of 20.     

Separation of the radioelements210Pb−210Bi−210Po by spontaneous deposition onto noble metals and verification by Cherenkov and liquid scintillation counting

A method for the separation of²¹⁰Pb,²¹⁰Bi and²¹⁰Po using spontaneous deposition has been developed. The²¹⁰Bi and²¹⁰Po are simultaneously removed by deposition onto nickel foil (copper and tin could also be used but less effectively) while the²¹⁰Po is separated from²¹⁰Bi, after dissolution of the nickel foil, by deposition onto silver foil. The effectiveness of each separation was evaluated by adding aliquot portions of each solution to a cocktail and counting with a liquid scintillation counter. Water was used as the medium to observe the Cherenkov count of the sample solution.     

Simultaneous measurements of cosmogenic radionuclides <Superscript>32</Superscript>P, <Superscript>33</Superscript>P and <Superscript>7</Superscript>Be in dissolved and particulate forms in the upper ocean

A technique to determine concentrations of ³²P, ³³P and ⁷Be in dissolved and particulate forms, in the upper ocean was developed. By using a large volume in situ filtration and concentration system (LV-FiCS), several tons of seawater at different depths were filtered concurrently through two kinds of filters. The dissolved radionuclides were concentrated onto adsorbents in the LV-FiCS. The radionuclides obtained were further purified by precipitation and ion-exchange chromatography, and quantified by gamma-spectrometry and ultra-low level liquid scintillation counter measurements. The technique was used with good results in a coastal area of Ibaraki, Japan.     

Counting efficiency and colour quenching in measuring Cherenkov radiation

The counting efficiency of Cherenkov radiation by the liquid scintillation counter is studied in several solvents. The relation between the strength of the pulse height by the Cherenkov radiation and the maximum energy of -rays was fairly proportional. The colour quenching can be corrected by measuring the absorbance of solution.