Ultra-sensitive determination of K, Th, U and other trace impurities in liquid organic scintillators by NAA

We present a NAA method to determine ultratraces of K, Th, U and other trace impurities in liquid organic scintillators, which are known as ultrapure detector materials for neutrino or dark matter experiments. A combined optimization of relevant factors for sensitive NAA has been realized, leading to a sensitivity for U down to 10⁻¹⁶g/g. Samples of 250 ml have been irradiated up to 120 h at a thermal neutron flux of 5–8·10¹²·n·cm⁻²·s⁻¹. Acidic extraction, wet ashing and TBP-extraction are used for radiochemical separations. Finally, coincidence techniques are applied for increased sensitivity.     

Fast-neutron activation analysis with short-lived nuclides

At the GKSS Research Center Geesthacht, a new 14 MeV activation facility—a 5·10¹² n/s neutron generator combined with a fast rabbit system (KORONA)—is being installed. Homogeneous neutron flux at a level of 5·10¹⁰ n·cm⁻²·s⁻¹ and sample transfer times of 140 ms to a 16m distant detector station are characteristic features of the facility described in the paper. With special consideration of short-lived nuclides and including cyclic activation, the analytical prospects with the intense neutron source are discussed, and sensitivities for 78 elements are presented.     

The determination of tin in rocks by thermal neutron activation

A fast routine method for the determination of tin in rocks is discussed. The method is based on coprecipitation of tetravalent tin with ferric hydroxide, followed by a short irradiation in a high thermal neutron flux, extraction in toluene from 1∶1 sulphuric acid which is 5N in potassium iodide, and counting of^123mSn (T=40 m) or^125mSn (T=9.7 m) with a well-type NaI detector. In the present work^125mSn was used. The lower limit of determination is governed by the blank of the reagents. For a sample of at least one gram it is ≌ 0.2 μg Sn·g⁻¹.     

Activation of Tl,Pb and Bi by 10–160 MeV neutrons: Possible application to the analysis of Bi+

The medium energy intense neutrons (MEIN) available at the Brookhaven Chemistry Linac Irradiation Facility have an energy distribution up to ∼160 MeV an effective neutron flux of ∼1.3×10¹¹ cm⁻²s⁻¹. The present work explores the feasibility of using this facility for the analysis of Tl, Pb and Bi by activation with MEIN. The most sensitive reactions, from a practical standpoint, were found to be Tl (n, xn)²⁰⁰Tl (x=4, 6), Pb (n, xn)^204mPb (x=0, 3, 4. 5) and²⁰⁹Bi (n, 6n)²⁰⁴Bi. The absolute sensitivities attainable with these reactions are 0.1, 0.05 and 0.08 μg of Tl, Pb and Bi respectively, for 1 h irradiation at 1.3×10¹¹ n cm⁻²s⁻¹ with samples counted 2 h after the end of irradiation. The advantages of the method over thermal neutron activation analysis are that all three elements can be assayed at the sub-microgram concentration levels by γ-spectrometry with the help of a simple radiochemical purification and the analytical results can be verified by cross checking via the multiple (n, xn) reaction products. However, interference from Bi in the determination of Pb and from Pb and Bi in the determination of Tl limits its usefulness to the analysis of Bi. This research was sponsored under contract with the United States Department of Energy supported by its Office of Basic Energy Sciences (support for H.L. FINSTON is under Contract no. DE-AC02-76-ER03126).     

Rare-earth elemental analysis of banded iron-formations by instrumental neutron activation analysis

Representative banded iron-formations (BIFs) from various locations of the eastern Indian geological belt were investigated by instrumental neutron activation analysis (INAA). After pre-concentration, irradiation was carried out using a neutron flux of 5.1·10¹⁶ m⁻²·s⁻¹, 1.0·10¹⁵ m⁻²·s⁻¹ and 3.7·10¹⁵ m⁻²s⁻¹, with thermal, epi-thermal and fast neutrons, respectively. The activities in these samples were measured by a HPGe detector. Ten rare-earth elements, such as La, Ce, Nd, Sm, Eu, Tb, Ho, Tm, Yb and Lu, have been qualitatively identified and quantitatively estimated in these samples. The present investigation is an example of employing a pre-concentration method for high iron-containing ores prior to neutron activation analysis.     

Determination of phosphorus in polymers by INAA

An INAA technique employing beta spectrometry was developed for the determination of phosphorus in polymers. The (n,γ) reaction on phosphorus produces³²P, half-life 14.3 days, a pure beta emitter with end-point energy 1.71 MeV. Polymer samples in the form of powders, films and pellets are irradiated and then counted with a plastic scintillator. The beta spectrum is corrected for interferences (especially Sb, Zn and Br which are quantified by gamma spectrometry) and for energy loss in the thick sample. Samples must also be analyzed for S and Cl which cause nuclear interferences. With an irradiation time of 4 hours at a neutron flux of 5·10¹¹ n·cm^{−2 s −1}, decay time 10 days and counting time 10 minutes, the sensitivity is 520 counts/μg phosphorus and the detection limit is typically 2μg/g.     

A brief introduction to NAA facilities of China Advance Research Reactor at CIAE

China Advance Research Reactor (CARR) at China Institute of Atomic Energy (CIAE), with a non-perturbed maximum thermal neutron flux of 1 × 10¹⁵ cm⁻² s⁻¹ at the center of active area, is one of the most powerful research reactors in the world. Three neutron channels have been allocated for conventional neutron activation analysis (NAA), thermal neutron prompt gamma activation analysis (PGAA) and cold neutron PGAA, respectively. Two irradiation tube systems are installed in the conventional NAA channel. One of them is for short irradiation with the rabbit size of diameter (Φ)19 × 40 mm, the other one is for long irradiation with the rabbit size of Φ39 × 70 mm. The medium temperature is about 45 °C and the thermal neutron flux is about 3 × 10¹⁴ cm⁻² s⁻¹ at sample positions. The flux gradient is expected to be very small according to the designed neutron flux distribution. Pneumatic systems are used for samples transfer. The speed of rabbits is designed to be about 20 m/s, and it takes 3 s to travel from irradiation position to detector. Three sets of gamma counting systems and one delayed neutron counting system are being equipped for routine analysis. They are designed for running continuously and automatically. And all the functions can be operated at laboratory or office through remote controlled computer. Software has been made domestically for spectrum peak search, concentration calculation with relative method and k₀ method with interference corrections and some other functions for the convenience of users.     

Concentrations of trace and major elements in Mission–Progresso (Texas) soils

Neutron Activation Analysis (NAA) was applied to determine trace and major elements in Mission–Progresso (Texas) soils. The Rio Grande river runs along the USA—Mexico border. The soil samples were collected at Mission and Progresso areas of the Rio Grande riverbank in the USA side. Soils were analyzed for the presence of toxic effluents due to human activities that might affect agricultural products and health because one of the possible paths of intoxication is the agricultural product consumption. Dried, sieved, and blended soil samples (~1.5 g) were irradiated at the UT Austin TRIGA reactor at a thermal neutron flux of 1 × 10¹² n cm⁻²s⁻¹ and epithermal neutron flux of 1 × 10¹¹ n cm⁻²s⁻¹. Different irradiations, decay, and counting times were combined to determine concentration and detection limits of 21 elements which represent four areas in Mission–Progresso (Texas) with the aim to achieve a consistent characterization. NIST certified reference materials were used in relative analysis and also to determine the accuracy and reproducibility values. The neutron flux was monitored using sulfur flux monitor wires. Normal and Compton suppression gamma ray spectrometers were used to detect different gamma ray energy peaks and this Compton system greatly reduces the background. Concentrations are evaluated in per cent and parts per million and errors are within acceptable levels and these values are compared with values reported in literatures from other countries. The results do not show significant contaminations neither from the Rio Grande river nor from nearby industries.     

Test-fitting on adsorption isotherms of organic pollutants from waste waters on activated carbon

An alternative method of approach has been developed for the measurement of thermal neutron flux. The method depends only on the activity of the bare foil if the cadmium ratio at the irradiation position is known. The method has been tested on the GHARR-1 facility at the Ghana Atomic Energy Commission using gold and indium foils for the measurement of the thermal neutron flux in the flux range of 10¹⁰–10¹² n·cm⁻²·s⁻¹ and the results compare very well with those obtained using the conventional method (cadmium separation method).     

Evaluation of stray neutron distribution in medical cyclotron vault room by neutron activation analysis approach

Stray neutron distribution in a medical cyclotron vault room was evaluated by neutron activation analysis (NAA). Neutrons were generated in the production of radioactive nuclides, such as ¹⁸F, ¹¹C, ¹³N and ¹⁵O, for diagnostic usage. Indium foil was adopted to evaluate the stray fast and thermal neutron intensity based on ¹¹⁵In(n_f, n′)^115mIn and ¹¹⁵In(n_th, γ)^116m1In reactions, respectively. The indium foils were weighed, sealed and placed at 62 points around the 6.7×8.2 m² cyclotron room. Additionally, each indium foil was exposed for over 80 minutes during cyclotron operation and γ-peaks were analyzed using an HPGe detector to evaluate the number of stray fast (Φ _f) or thermal (Φ _th) neutrons. The minimum to maximum numbers of fast and thermal neutrons were (3.47±0.11)×10³ to (1.06±0.21)×10⁴ n·cm⁻²·s⁻¹ and 9 to 965 n·cm⁻²·s⁻¹, respectively. The minimum detectable limit for stray neutrons was included herein to demonstrate the reliability. Accordingly, 60 and two points, respectively, the confidence level associated with the reported intensities of fast and thermal neutrons reached 95%. The low qualified ratio in the evaluation of stray thermal neutrons might have been caused by either the high Compton scattering plateau or the low intensity of the gamma-ray peak in the relevant spectrum.     

Alternative chromatographic processes for no-carrier added 177Lu radioisotope separation Part I. Multi-column chromatographic process for clinically applicable

The conventional multi-column solid phase extraction (SPE) chromatography technique using di-(2-ethylhexyl)orthophosphoric acid (HDEHP) impregnated OASIS-HLB sorbent based SPE resins (OASIS-HDEHP) was developed for the separation of no-carrier added (n.c.a) ¹⁷⁷Lu from the bulk quantity of ytterbium target. This technique exploited the large variation of lutetium metal ion distribution coefficients in the varying acidity of the HCl solution-OASIS-HDEHP resin systems for the consecutive loading-eluting cycles performed on different columns. The production batches of several hundred mCi n.c.a ¹⁷⁷Lu radioisotope separated from 50 mg Yb target activated in a nuclear reactor of medium neutron flux (Φ = 5·10¹³ n·cm⁻²·s⁻¹) were successfully performed using the above mentioned separation technique. With the target irradiation in a reactor of thermal neutron flux Φ = 2·10¹⁴ n·cm⁻²·s⁻¹ or the parallel run of several separation units, many Ci-s of n.c.a ¹⁷⁷Lu can be profitably produced. The OASIS-HDEHP resin based multi-column SPE chromatography technique makes the separation process simple and economic and offers an automation capability for operation in highly radioactive hazardous environments.     

The determination of fluorine in bones by non-destructive neutron activation analysis using 11.2 sec20F

A fast non-destructive determination of fluorine in bone samples by thermal neutron activation analysis using¹⁹F(n, γ)²⁰F reaction was developed. About 0.1–1 g samples is irradiated for 15 sec in TRIGA MARK II reactor at a thermal neutron flux of 5·10¹¹ n·cm⁻²·sec⁻¹. After 15–25 sec cooling, the 1633 KeV²⁰F activity (T=11.2 sec) is counted for 15 sec with a Ge(Li) spectrometer. A standard sample is prepared by mixing CaF₂ and CaCO₃ powders. The interference from²³Na(n, α)²⁰F is corrected by employing²⁴Na 2754 KeV double escape peak activities in samples and the²⁰F/²⁴Na peak area ratio observed previously for pure Na₂CO₃ powder. The precision is 7% for a bone sample containing 1020 ppm F and the sensitivity is about 10 ppm F.     

Analysis of phosphate rock samples for vanadium using accelerator-based thermal neutrons

Extensive sedimentary phosphate deposits exist in the Sirhan-Turayf basin in northwestern Saudi Arabia containing significant amounts of uranium, thorium, vanadium and rare earth elements. The determination of the concentration and pattern of distribution of some of these elements is essential for economic aspects. This study reports the analysis of vanadium in selected phosphate rock samples from the basin using accelerator-based thermal neutrons activation analysis (TNAA). Samples were irradiated in a thermal neutron flux of 2.5·10⁶ n·cm⁻²·s⁻¹. The induced activity was measured with a HP-GMX detector coupled to a PC-based data acquisition and analysis system. The facility was calibrated using certified standards of vanadium. The minimum detection limit of vanadium was about 1 mg. Three independent measurements on each sample yielded comparable results indicating the reliability of the technique. The vanadium concentrations in the samples vary from 23 to 457 ppm. This revised version was published online in July 2006 with corrections to the Cover Date.     

Aktivierungsanalytische Bestimmung von Nickel in Ionenaustauschern

A method for the determination of nickel in ion exchange resins has been elaborated. It is based on the⁵⁸Ni(n, p)⁵⁸Co reaction. Samples of 500 mg are irradiated for 90 h in a fission neutron flux of 10¹³ n·cm⁻²·s⁻¹. After decomposing by HNO₃/HClO₄ mixture the radiochemical separation is carried out by extraction of the Co-DDTC-complex in chloroform. Measuring by a 23 cm³ Ge(Li) detector for 15 h provides a detection limit of 10 ppb. Radiochemical yield is determined by⁵⁷Co as radioactive indicator. Limitations by⁶⁰Co are reduced by Cd-screened activation and by anticoincidence measuring technique.      

Determination of lithium by instrumental neutron activation analysis

The fast transfer system in the DR 2 reactor for irradiation at a thermal neutron flux density of 10¹³ n·cm⁻²·sec⁻¹ was used for the determination of lithium by the⁷Li(n, γ)⁸Li reaction. β-counting with a large perspex Cerenkov detector begun at 0.3 s after the end of irradiation, and multi-scaler data was accumulated in 300 channels at 0.1 s per channel. With a suitable choice of discrimination level only¹⁶N and background interfere, and the 0.84 s half-life of⁸Li was resolved by the method of weighted least squares. Results are presented for 36 international geochemical reference materials, and for a few biological samples, including BOWEN's kale and the NBS Standard Reference Material 1571 Orchard Leaves.     

Characterization and use of the new NIST rapid pneumatic tube irradiation facility

Recently a new rapid pneumatic tube facility was inserted into a long unused location in the NIST 20 MW nuclear reactor. This facility was designed and constructed specifically for rapid INAA using short lived activation products. Included is a computer controlled console which uses fast sensors to accurately measure the irradiation capsule flight time, and a loss-free counting system connected to a 32% efficient PHGe detector with a transistor reset preamplifier. Measurement of travel, times from end-of-irradiation to detector were 473±8 ms. Measurement of the thermal neutron fluence rate was 5.0·10¹³ n·cm⁻²·s⁻¹. The other three pneumatic tubes in the NIST reactor have transfer times of 3 to 15 seconds, and no timing capability more accurate than human response. This new facility substantially improves our ability to accurately determine activation products with half-lives from 1 to 100 seconds. Characterization information reported on this new irradiation facility includes absolute fluence measurements, fluence rate variations within the capsule and variations with time, and determination of analytical sensitivities for fluorine-20 selenium-77m, and silver-110g.     

Activation analysis of selenium in organic samples,through selenium-77m,on a pre-separation basis

A method is described to separate trace amounts of selenium in organic samples without using a carrier, based on the adsorption on active carbon filters of the complex formed with APDC at pH 1.5. The separation is made prior to the neutron irradiation and the correction for selenium in the reagents performed by the irradiation of a blank. The method has been successfully used in fodder samples as well as some other organic reference materials, using a fast pneumatic transfersystem, which takes the samples from the irradiation position to the counting position in 3s, with the only limitation of the thermal neutron flux available, 4.7·10¹¹ cm^–2·s^–1. Detection limits of 0.1 g are obtained under these experimental conditions.     

Halogen speciation in the rat thyroid: Simultaneous determination of bromine and iodine by short-term INAA

The study describes a mode of non-destructive simultaneous determination of bromine and iodine concentrations, by reactor instrumental neutron activation analysis (INAA) in the regime of short-term activation. Under the conditions of 1-minute activation in the neutron flux of 8.0·10¹³ n·cm⁻²·s⁻¹, it was possible to determine reliably as little as 5·10⁻⁸ g bromine and about 10⁻⁷ g iodine in matrices of a given type and of the mass of about 5 mg dry weight. We applied this method for the determination of Br and I concentrations in the whole rat thyroid gland as well as for the halogen speciation in fractions separated from this organ.     

Multi-element analysis of biological samples after intense neutron irradiation an fast chemical separation

For the simultaneous determination of many elements in small biological samples, a multi-element analysis has been developed using neutron activation. After a 24-hr irradiation in a neutron flux of 2.5·10¹⁴ n·cm⁻²·sec⁻¹ and after immediate chemical separation without cooling, it was possible to analyse 24 elements in bovine liver (NBS-SRM 1577). The separation apparatus, set up in a shielded cell can work four samples simultaneously, and its operation is fast enough to allow the detection of radioisotopes with a half-life of about 2 hrs (¹⁶⁵Dy,^57mSr,⁵⁶Mn). Amounts lower than 10⁻³ μg of Dy, Eu, Pr, Sm and Yb were determined.