Development of an elemental tracer using neutron activation analysis for application in an estuarine environment

Summary The work describes the selection of an activable tracer that could be used to study dispersion patterns in an English estuary and was carried out in connection with the development and testing of a particle-tracking computer model. Understanding estuarine dynamics will assist in the decision-making process for estuarine management and in contingency planning. Neutron activation analysis (NAA) has been used to characterize the concentration and natural variation of 40 trace elements in suspended particulate matter and inter-tidal bed sediment in order to identify a suitable tracer. Results have shown that europium, terbium and ytterbium would be suitable to use in a tracer study as they have low background concentrations in sediments and little variability, (Eu: 1.31 mg ^. kg^-1±13%, Tb: 0.90 mg ^. kg^-1±16% and Yb: 2.91 mg ^. kg^-1±18%). The ratios of these elements are constant throughout the estuary and experiments have shown that increases in concentration of any of these elements due to the addition of artificial elemental tracer could be quantitatively determined by changes in the ratio constant.     

81mSe tracer for determination of the chemical yield in radiochemical neutron activation analysis of selenium

A radiotracer method is described for measurement of the chemical yield in radiochemical neutron activation analysis of selenium using the⁷⁵Se (120 d) induced nuclide. It is based on^81mSe (57 min) radioisotopic tracer, prepared immediately before its use in the radiochemical separation procedure, by neutron irradiation of highly enriched⁸⁰Se. The recovery of selenium is calculated from the 103 keV -peak of^81mSe in the separated selenium fraction used for quantitation of⁷⁵Se. The technique is illustrated by results for biological reference materials of good accuracy and reproducibility.     

Prompt-gamma neutron activation analysis using an isotopic neutron source

This paper describes an experimental set up using an isotopic neutron source with graphite, preferably to a hydrogen-rich compound, as moderator. This low thermal flux source has been employed in PGNAA experiments. Only those elements having a high cross section can be quantitatively analyzed at low concentration levels, mainly, Gd, Cd, Sm, B and Hg; the other elements can only be probed at macroscopic levels. An application to the determination of boron content in collyria examplifies the possibilities of the technique.     

156Dy as an activable yield tracer for determination of rare earth elements in biological materials by neutron activation analysis

Use of an enriched¹⁵⁶Dy isotope as an activable yield tracer for the determination of lanthanoid contents in various biological reference materials has been proposed. The method consists of preconcentration of the lanthanoid in the¹⁵⁶Dy doped samples followed by neutron irradiation and further chemical purification steps. The chemical behaviour of lanthanoid elements in the whole procedure was found, in separate runs, similar to that of the added¹⁵⁶Dy within experimental errors. Simple purification steps after irradiation allow the measurement of relatively short-lived nuclides and diminish the radiation dose received during the chemical treatment. The present results for orchard leaves (NBS SRM 1571) are generally in good agreement with the previously reported data. Some new data are obtained for other biological reference materials.     

Application of the radioreagent method for yield determination in neutron activation analysis

A very convenient method for yield determination in NAA is the use of isotopic radiotracers. But for the majority of elements determinable by NAA no suitable isotopic radiotracers exist. For some of these elements the radioreagent methodoffers afvourable opportunity to use also non-isotopic radiotracers. An activation analytical copper determination method is described using a radioactively labelled reagent for correction of separation losses. Results of copper determinations in 8 international standard reference materials are given.     

Epithermal neutron activation analysis using the monostandard method

A method is described for epithermal neutron activation analysis of 17 elements in granite rock samples using a single standard. Gold has been used as a single comparator due to its relatively high resonance integral value (I₀=400 barn). In addition, it is preferable to Co in order to obtain a large epithermal activation in a short irradiation. The method of calculation is simple and rapid and can be done using a small calculator. Epithermal activation is able to overcome the difficulty arising from changing irradiation position as well as increasing the number of determinable elements by eliminating the interference from undesired isotopes which have relatively high thermal cross section values (₀), when reactor neutron flux is used. The coupling of epithermal activation with the monostandard method has the advantage of using a small Cd-cover which overcomes most of the difficulties arising in the relative method with large volume cadmium filters.     

Thermal and epithermal neutron activation analysis using the monostandard method

A new approach is presented for neutron activation analysis using the monostandard (single comparator) method. Elements to be determined are classified into two groups; those with σ_o>I_o are activated with whole neutron spectrum (without Cd-cover), using a standard of the same group (e.g. Sc), while elements with I_o>σ_o are activated with epithermal neutrons (under Cd-cover) using a standard of the same group (e.g. Au or Co). Epithermal activation increases the number of determinable elements and its coupling with the monostandard method has the advantage of using a small Cd-cover. The σ_o and I₀ values of some elements were determined to test this approach.     

Determination of the fast fission yield of141Pr using neutron activation analysis

A method is described for the determination of the fission yield of¹⁴¹Pr. This method was developed to determine the fast fission yield of¹⁴¹Pr in the Mark III loading (enriched uranium with about 2% zirconium) of the fast fission breeder reactor, EBR-1. The burnup of the fuel sample was determined using the previously reported fission yield of¹³⁷Cs. Praseodymium was separated from uranium, plutonium and other fission products by a combination of precipitation and ion exchange stages. Thereafter,⁵⁵Mn was added to serve as an internal flux monitor and praseodymium determined by neutron activation analysis. A precision of ±2% was obtained. Presented at the 15th Annual Meeting of the American Chemical Society, Miami Beach, Florida (USA), April 1967.     

Enriched uranium as an activatable tracer in environmental research

Isotopically enriched uranium and delayed neutron assay have been employed to study uranium dynamics within bee colonies. Preliminary data demonstrating the advantages of this activatable tracer method are presented.     

Multi-elemental epithermal neutron activation analysis using an internal single comparator

Epithermal neutron activation analysis using an internal single comparator has been used for the analysis of Saudi Arabian iron ores. The concentration of thorium, barium, terbium, tantalum, cobalt, lanthanum and antimony was determined using iron in the ore as an internal comparator for all the elements. In case of antimony there was an agreement between this method and the conventional method indicating that the given method is accurate.     

Instrumental neutron activation analysis of geological and pedological samples. Further investigation of epithermal neutron activation analysis using monostandard method

A comparative study is presented on neutron activation analysis of rock and soil samples using whole reactor neutron spectrum and epithermal neutrons with both relative and monostandard procedures. The latter procedure used with epithermal neutron activation analysis of soil samples necessitated the use of the “effective resonance integrals” which were determined experimentally. The incorporation of the β factor, representing deviation of reactor epithermal neutron flux from 1/E law, is developed in the present work. The main criteria for the choice of one or more of the procedures studied for a given purpose are also indicated. Analysis of 15 trace elements, Ca and Fe in the standard Japanese granite JC-1 using monostandard epithermal neutron activation gave results in good agreement with the average literature values. This paper is dedicated to the 80th birthday of Professor Dr. Robert Klement, University of Munich.     

Instrumental neutron activation analysis of environmental samples using thek 0-standardization method

The use of thek ₀-standardization method in instrumental neutron activation analysis gives good accuracy and precision. The analysis time can be reduced drastically by employing software for thek ₀-standardization calculations. In this work samples were irradiated in a TRIGA reactor and the gamma spectrum was analysed by Sampo 90 and thek ₀-standardization by the KAYZERO/SOLCOI code (DSM Research). The efficiency measurement and the peak to total ratio at the reference and other geometries were measured and tested for their accuracy by analysing some reference materials. Reference materials such as SRM 1572 (Citrus leaves), SRM 1573 (Tomato leaves), SRM 1575 (Pine needles), IAEA Soil-7 (Soil) and SRM 1646 (Estuarine sediment) were analysed for the major, minor and trace element contents. The results were in good agreement with the certified or literature values. The recently released IAEA 140 (Sea plant homogenates) was also analysed for 28 elements.     

Fast neutron activation analysis using short-lived radionuclides

Fast neutron activation analysis experiments were performed to investigate the analytical possibilities and prospective utilization of short-lived activation products. A rapid pneumatic transfer system for use with neutron generators has been installed and applied for detecting radionuclides with a half-life from 300 ms to 20 s. The transport time for samples of total mass of 1–4 g is between 130 and 160 ms for pressurized air of 0.1–0.4 MPa. The reproducibility of transport times is less than 2%. The employed method of correcting time-dependent counting losses is based on the virtual pulse generator principle. The measuring equipment consists of CAMAC modules and a special gating circuit. Typical time distributions of counting losses are presented. The same 14 elements were studied by the conventional activation method (single irradiation and single counting) by both a typical pneumatic transport system (run time 3 s) and the fast pneumatic transport facility. Furthermore, the influence of the cyclic activation technique on the elemental sensitivities was investigated.     

Development of an automatic system for neutron activation analysis

An automatic measurement system for activation analysis has been developed at the La Reina Nuclear Center of the Chilean Nuclear Energy Commission. A gamma-ray spectrometer equipped with an automatic sample changer is linked to an IBM-compatible PC/AT. The peripheral devices are interconnected and suitable software for routine operation have been prepared. The computer handles solenoid valves and microswitch sensors. The gamma-spectra are stored in the hard disk and later transferred to a main frame computer where all the information is processed to obtain final results. The system is in full operation and the operation manuals that have been prepared allow it to be used by people who are not trained in activation analysis.     

Enriched copper isotope tracer for dietary copper incorporation into hair using neutron activation analysis in conjunction with direct-current argon plasma spectrometry

A method is described for labeling and measuring the incorporation of dietary copper into hair using the enriched (99.61 atomic-%) ⁶⁵Cu isotope. Natural isotope abundant copper exists as ⁶⁵Cu (30.86 atomic-%) and ⁶³Cu (69.17 atomic-%), but enriched (99.61 atomic-%) ⁶⁵Cu isotope may be obtained commercially and administered to change deliberately the natural isotope abundance of copper to “label” the copper source. Natural isotope abundant copper and the enriched (99.61 atomic-%) ⁶⁵Cu isotope were mixed into rat feed and administered daily by gavage. The isotope concentration was determined by neutron activation analysis (NAA). The copper concentration was determined by direct-current argon plasma (DCP) spectrometry.The measured copper isotope ratios (⁶⁵Cu/Cu_tot)_for the natural isotope abundant copper in National Bureau of Standards Standard Reference Materials (NBS SRM) 1571 Orchard Leaves and 1577a Bovine Liver were 0.3201 ± 0.0039 and 0.3187 ± 0.0089, respectively. Measured copper isotope ratios in rat hair were 0.3100 ± 0.0606, 0.4580 ± 0.2495 and 0.2712 ± 0.0645 from rats given a standard feed that contained natural isotope abundant copper, a daily supplement of natural isotope abundant copper sulfate mixed into the standard feed and a daily supplement of copper sulfate administered by gavage, respectively. The copper isotope ratio increased to 0.5251 ± 0.2860 and 0.7235 ± 0.0704 in hair from rats given enriched ⁶⁵Cu in their feed and by gavage, respectively. The statistically significant increase in the ⁶⁵Cu isotope when administered by gavage demonstrates strates successful labeling of dietary copper in the hair.     

Instrumental neutron activation analysis technique using subsecond radionuclides

The fast irradiation facility Mach-1 installed at the Danish DR 3 reactor has been used in boron determinations by means of Instrumental Neutron Activation Analysis using¹²B with 20-ms half-life. The performance characteristics of the system are presented and boron determinations of NBS standard reference materials as well as fertilizer materials are compared by literature value and spectrophotometric measurements, respectively. In both cases good agreement is obtained.     

The study of human nails as an intake monitor for arsenic using neutron activation analysis

Arsenic is toxic to humans with the lethal dose being approximately 1 mg/kg/day. At much lower long-term exposures, arsenic is hypothesized to increase the risk of certain cancers. We have developed an irradiation position for the neutron activation analysis (NAA) of nail specimens for arsenic, in support of a case-control study involving New Hampshire residents consuming well water above the EPA Safe Drinking Water Standard of 0.050 ppm. Arsenic is bound to nail keratin through sulfhydryl groups proportional to intake providing a convenient means of integrating arsenic intake in population-based studies. Our objective was to develop the necessary facilities and procedures by which relatively small samples (i.e. 20 to 100 mg) could be accurately analyzed for arsenic, so that affordable nutritional epidemiology investigations, requiring large numbers of samples (>1000 in this case), could be undertaken. A high-flux reflector position, with minimal axial variation throughout the fuel cycle, suitable for pneumatic-tube irradiations, was characterized by measurement of the neutron flux distribution (thermal and epithermal) within the irradiation capsule over time. Results from application of the method to a case-control study of basal and squamous cell skin cancer will be presented.     

Determination of cadmium using radiochemical neutron activation analysis

A method has been developed for the determination of cadmium in samples of food and biological materials using neutron activation analysis with radiochemical separation. The irradiated sample is digested in presence of cadmium carrier, with a nitric-perchloric mixture, evaporated to dryness, dissolved in 6M HCl and placed onto an ion exchange column loaded with Dowex 1-X8 resin in chloride form and conditioned with HCl 6M. The cadmium is retained in the resin. After a washing procedure with several portions of HCl of decreasing concentration, the cadmium is eluted with an ammonia-ammonium chloride buffer. The activity of ^115mIn which is in equilibrium with ¹¹⁵Cd, is measured using a NaI(Tl) well type detector. The method has been evaluated by analyzing certified reference materials with cadmium concentrations covering a range of 0.020 to 200 mg^.kg^-1. The agreement of the results with the certified values is within 95%, which gives an indication of the sensitivity and accuracy of the proposed method.     

14 MeV neutron activation analysis using short-lived products

Cyclic activation using pneumatic shuttling system and switch off and on the neutron source and detector are described in order to eliminate some uncertainties by the provision of more accurate timing, the measurement of the effective activating neutron flux and the correction for the detection system dead time.     

A complex neutron activation method for the analysis of biological materials

The aim of the present work was to deal primarily with a few essential trace elements and to obtain reliable results of adequate accuracy and precision for the analysis of biological samples. A few other than trace elements were determined by the nondestructive technique as they can be well evaluated from the gamma-spectra. In the development of the method BOWEN's kale was chosen as model material. To confirm the reliability of the method two samples were analysed proposed by the IAEA in the frame of an international comparative analysis series. The comparative analysis shows the present method to be reliable, the precision and accuracy are good.