Using synthetic multi-element standards (SMELS) for calibration and quality control of the irradiation facilities in the BR1 reactor

The thermal to epithermal neutron flux ratio (f) and the deviation of the epithermal neutron spectrum from the 1/E shape (α) are essential parameters for the correct application of k ₀-standardized neutron activation analysis. Several methods are applied for the determination of f and α. They are based on Cd-covered multi-monitor or on bare-irradiations methods. The recently developed and characterized synthetic multi-element standards (SMELS) were designed as a validation tool for the proper implementation of the k ₀-NAA method in a laboratory. In particular, SMELS Type III contains Au and Zr, thus allowing the direct determination of f and α. It could, therefore, replace the traditional flux monitors. Furthermore, it could be used as a quality control material to monitor the stability of the irradiation facility and the detector. This paper presents the accuracy of the f and α determination and the feasibility of quality control using SMELS for irradiation channel Y4 of the BR1 reactor.     

Characterization of pneumatic fast transfer system irradiation position of KAMINI reactor for k 0-based NAA

The pneumatic fast transfer system position at KAMINI reactor, Indira Gandhi Centre for Atomic Research, India was characterized by determining the epithermal neutron flux shape factor (α) and the sub-cadmium to epithermal neutron flux ratio (f) for k ₀-based Neutron Activation Analysis (k ₀-NAA). For determination of α value, bare, Cd-ratio and Cd-cover methods were employed using dual and multi monitors namely Au, Zr and Zn. For calculation of f, Au and Zr monitors were used in the case of bare method and Au monitor was used for cadmium ratio and cadmium cover methods. The determined α-value of PFTS indicated a hard epithermal neutron spectrum and the f value indicated about 96 % thermal neutron component. For validation of k ₀-NAA method, reference materials namely NIST SRM 1646a (Estuarine Sediment) and BCS Nb-stabilized Stainless Steel (BCS/SS No.261/1) were analyzed. The percentage errors of the determined concentration values of elements were within ±5 % with respect to the certified values and the Z-score values at 95 % confidence level were within ±2 in most of the cases.     

Implementation of <Emphasis Type="Italic">k</Emphasis><Subscript>0</Subscript>-standardization method of the INAA at ETRR-2 research reactor

The k ₀-method of INAA standardization has been implemented using the irradiation facilities of the fast pneumatic rabbit and some selected manually loaded irradiation positions, which designated for short and long irradiation, respectively, at Egypt second research reactor. The neutron flux parameters (f and α) in each site have been determined using Zr–Au sets as neutron flux monitors. The reference materials coal NIST 1632c and IAEA-Soil 7 were analyzed for data validation and good agreement between the experimental values and the certified values was obtained.     

Experimental and MCNP calculations of neutron flux parameters in irradiation channel at Es-Salam reactor

The Algerian research reactor (Es-Salam) is a 15 MW heavy water reactor type, operating since 1992. It became essential to characterize the neutron field in the most useful irradiation positions, in order to guarantee the accuracy in the application of k ₀-neutron activation analysis (k ₀-NAA). Experimental value of the thermal to epithermal neutron flux ratio (f) and of the deviation of the epithermal neutron spectrum from 1/E shape (α) were determined using different methods. This work focuses the verification of Monte Carlo neutron flux calculation in typical irradiation channel. Comparison of the results for parameter f obtained experimentally and by Monte Carlo simulations shows good agreement in the irradiation channel studied. The difference between both results is about 2.08%.     

Cation distribution in Ni-substituted Mn-ferrites by Mössbauer technique

The neutron spectra of one outer (#10) and two inner (#2 and #3) sites of the Dalhousie University SLOWPOKE-2 reactor (DUSR) have been calibrated for the k ₀-based neutron activation analysis (k ₀-NAA). The parameters determined include the cadmium ratio (R _Cd), epithermal neutron flux shape factor (), subcadmium-to-epithermal neutron flux ratio (f), thermal-to-fast neutron flux ratio (f _F), modified spectral index r()(T_n/T₀)^1/2, Westcott g _Lu(T _n)-factor, and absolute neutron temperature (T _n). The a-values of -0.0098±0.0045 and -0.0425±0.0047 and -0.0422±0.0053 and f-values of 57.1±2.2 and 18.8±0.4 and 18.9±0.4 were obtained for the sites #10, #2 and #3, respectively. The modified spectral index (MSI), g _Lu(T _n)-factor, and T _n have been determined for the handling of non 1/v (n,) reactions. The accuracy of the method was evaluated by analyzing reference materials.     

Photoneutrons from a beryllium reflector: a potential source of problems with Zr–Au flux monitors in <Emphasis Type="Italic">k</Emphasis><Subscript>0</Subscript> standardization based neutron activation analysis

The assumption that the shape of the epithermal neutron spectrum can be described, in any research reactor, by the 1/E ^1+α function is a fundamental starting point of the k ₀ standardization. This assumption may be questioned from a reactor physics viewpoint. The type of moderator, the existence of neutron reflectors, the additional production of (γ, n) neutrons and resonance capture by construction materials may be different for each reactor, with consequences for the shape of the neutron spectrum. This dependency may explain that various practitioners reported contradicting experiences with the use of Zr–Au flux monitors for the determination of the α-parameter. An objective view on the influence of the design of the reactor and irradiation facility on the shape of the neutron spectrum can be obtained by modeling. This has been applied in the Reactor Institute Delft for reactor configurations in which the irradiation facilities face the fuel elements with the presence of beryllium reflector elements. The Monte Carlo calculations indicate a distortion of the 1/E ^1+α relationship at the higher energy edge of the epithermal neutron spectrum. This distortion is attributed to the formation and thermalisation of both photoneutrons and (n, 2n) produced fast neutrons in the beryllium, and has a direct impact on the resonance activation of ⁹⁵Zr, other than represented by the 1/E ^1+α function. The obtained relationship between neutron flux and neutron energy was also used for estimating the f-value and compared with the value obtained by the Delft Cr–Mo–Au flux monitor.     

Variation in k0 neutron flux parameters after replacement of the beryllium reflector and graphite wedge at the University of Missouri Research Reactor

In January 2006 the beryllium reflector and graphite wedge that contained the k₀ INAA irradiation position were replaced at the University of Missouri Research Reactor. Prior to replacement the average values of the flux ratio, f, and the epithermal non-ideality factor, α, were 57.4 ± 4.5 and 0.039 ± 0.012. The values of f and α immediately after the beryllium and graphite wedge replacement were 39.4 ± 0.6 and 0.021 ± 0.002. Subsequent measurements indicate that the neutron spectrum hardened with time, possibly due to the buildup of the ⁶Li atom density to saturation.     

Establishing a basis for nuclear archaeometry in Australia using the 20 MW OPAL research reactor

The k ₀-method of standardisation for instrumental neutron activation analysis (INAA) has been used at the OPAL research reactor to determine the elemental composition of three certified reference materials: coal fly ash (SRM 1633b), brick clay (SRM 679) and Montana soil (SRM 2711). Of the 41 certified elements in the three materials, 88 percent were within five percent of the certified values and all determinations were within 15 percent of the certified values. The average difference between the measured and certified values was 0.1 percent, with a standard deviation of 4.1 percent. Since these reference materials are widely used as standards in the analysis of archaeological ceramics by INAA, it has been concluded that the INAA facility in Australia is particularly well-suited for nuclear archaeometry.     

Development and implementation of <Emphasis Type="Italic">k</Emphasis><Subscript>0</Subscript>-INAA standardization at PINSTECH

The k ₀ method has been introduced at the 30 kW miniaturized neutron source reactor (MNSR) at the Pakistan Institute of Nuclear Science & Technology (PINSTECH). It involved the full energy peak efficiency calibration of the HPGe detector for different counting geometries and the characterization of the neutron flux at four inner irradiation channels. The latter involved the determination of the thermal to the epithermal flux ratio, epithermal flux shape factor, the modified spectral index, Westcott’s g-factor, the Maxwellian neutron temperature and the fast flux. The method was validated by analyzing IAEA-SL1 (Lake Sediment) and NIST-SRM-1572 (Citrus Leaves) reference materials. All calculations were performed in Excel, including the optimization step. The results revealed that most of the elements were estimated with less than 10% relative deviation from the certified value.     

Interacalation of pyridine and its derivatives into crystalline bismuth molybdenum hydrous oxide

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.     

Reactor power dependency of the neutron flux parameters fork 0-standardization

Using the facilities of the Triga Mark III reactor at the NNRI, Mexico and the HAV-1 multipurpose monitor, the reactor power dependency for thek ₀-standardization essential neutron flux parameters as: epithermal shape factor (), thermal to epithermal ratio (f) and neutron temperature (T _n ) were experimentally obtained. Evaluation of the obtained dependencies shows that it is unnecessary to analyze the possible introduction of correction factors in thek ₀-INAA experimental results. A single experimental procedure to determine throughf is suggested.     

Preparation and value assignment of standard reference material 968e fat-soluble vitamins, carotenoids, and cholesterol in human serum

Standard Reference Material 968e Fat-Soluble Vitamins, Carotenoids, and Cholesterol in Human Serum provides certified values for total retinol, γ- and α-tocopherol, total lutein, total zeaxanthin, total β-cryptoxanthin, total β-carotene, 25-hydroxyvitamin D₃, and cholesterol. Reference and information values are also reported for nine additional compounds including total α-cryptoxanthin, trans- and total lycopene, total α-carotene, trans-β-carotene, and coenzyme Q₁₀. The certified values for the fat-soluble vitamins and carotenoids in SRM 968e were based on the agreement of results from the means of two liquid chromatographic methods used at the National Institute of Standards and Technology (NIST) and from the median of results of an interlaboratory comparison exercise among institutions that participate in the NIST Micronutrients Measurement Quality Assurance Program. The assigned values for cholesterol and 25-hydroxyvitamin D₃ in the SRM are the means of results obtained using the NIST reference method based upon gas chromatography-isotope dilution mass spectrometry and liquid chromatography-isotope dilution tandem mass spectrometry, respectively. SRM 968e is currently one of two available health-related NIST reference materials with concentration values assigned for selected fat-soluble vitamins, carotenoids, and cholesterol in human serum matrix. This SRM is used extensively by laboratories worldwide primarily to validate methods for determining these analytes in human serum and plasma and for assigning values to in-house control materials. The value assignment of the analytes in this SRM will help support measurement accuracy and traceability for laboratories performing health-related measurements in the clinical and nutritional communities.     

k0-NAA quality assessment by analysis of different certified reference materials using the KAYZERO/SOLCOI software

A suite of natural matrix reference materials (RMs) were used to assess the quality of analytical results obtained by k ₀-instrumental neutron activation analysis (k ₀-INAA) at the Joef Stefan Institute (IJS). Five certified reference materials (CRMs) from the Institute for Reference Materials and Measurements (IRMM), two standard reference materials (SRMs) from the National Institute of Standards and Technology (NIST), three RMs from the International Atomic Energy Agency (IAEA) and one RM from IJS were analyzed. Altogether, results for twenty-four elements in inorganic matrices and twenty-nine elements in organic matrices, obtained by k ₀-INAA, were compared to certified values. Results obtained show good agreement with certified or assigned values except for Fe, La, Nd, Sm and U in inorganic matrices, and Ag, Al and Cr in organic matrices.     

Neutron spectrum calibration using the Cd-ratio for multi-monitor method with a synthetic multi-element standard

Several methods are in use for the determination of the thermal to epithermal neutron fluence rate ratio (f) and the deviation of the epithermal neutron spectrum from the 1/E shape parameter (α). In our former work, it was proven that the recently developed and characterized Synthetic Multi-ELement Standard (SMELS) can be used for the fast verification of the stability of the irradiation parameters using the Au-Zr bare monitor method. However, this latter method using SMELS had a too low precision for an accurate determination of f and α. Therefore, the Cd-ratio for multi-monitor method using SMELS was investigated for two irradiation channels. As shown the material can also be used as a monitor for the calibration of an irradiation facility.     

Determination of silver in biological reference materials by neutron activation analysis

Silver in selected, predominantly biological, reference materials (NIST SRM 1515, 1547, 1549, 1566a, 1571, 1577b, 2704, CTA-OTL-1, and Bowen’s Kale) was determined using neutron activation analysis (NAA) in two different analytical modes: instrumental NAA with epithermal neutrons (ENAA), and NAA with radiochemical separation (RNAA). The ENAA mode was based on long-time 5-hour irradiation of samples in a special Cd lined box with counting after 8-month decay. The RNAA procedure consisted in 20-hour irradiation of samples, their decomposition/dissolution by alkaline-oxidative fusion, and precipitation of AgCl including several purification steps. Both methods provided Ag contents in the analyzed reference materials consistent with certified and/or literature values down to the ng·g⁻¹ level.     

Neutron flux and associated k0 parameters in the RPI after the last configuration change

The Portuguese Research Reactor (RPI) is a 1 MW swimming pool type reactor, operating since the early 1960s. The fuel is MTR type, with flat plates of U-Al alloy enriched to 93% in ²³⁵U. As the core configuration changed in April 2000, it became essential to characterise the neutron field in the most useful irradiation positions of RPI, in order to guarantee the accuracy in the application of k ₀-neutron activation analysis (k ₀-NAA). Experimental values of the thermal to epithermal neutron flux ratio (f) and of the deviation of the epithermal neutron spectrum from the 1/E shape (a) were determined using the Cd-ratio for multi-monitor method. The neutron temperature (T _n) was obtained from co-irradiation of Lu with 1/v monitors. The results for several irradiation positions are presented and discussed in this work. Some element concentrations are determined based on the parameters obtained in this work, and compared with the certified reference material concentrations.     

The corrections for non-ideal behavior of the epithermal neutron spectrum and the restitution of the simplicity in parametric activation analysis

The errors occurred when α, the parameter that accounts for the non-ideal behavior of the epithermal flux, are neglected, have been evaluated for the determination of twenty elements in biological materials, using. gold and sodium comparators, and zirconium to measure the thermal to epithermal flux ratio (f). Sodium allows the determination of 15 elements, and up to 18 elements can be determined in positions relatively well thermalized by the simultaneous use of gold and sodium comparators, in all the cases with errors ≦2%, when α is not considered. Results obtained for reference materials are presented.     

Investigations on the comparator technique used in epithermal neutron activation analysis

The possible extension of the comparator technique of reactor neutron activation analysis into the field of epithermal neutron activation has been investigated. Ruthenium was used for multi-isotopic comparator. Experiments show that conversion of the so-called reference k-factors—determined by irradiation with reactor neutrons—into k_epi-factors usable at activation under cadmium filter, can be evaluated with fair accuracy. Sources and extent of errors and their contribution to the final error of analysis are discussed. Based on the paper presented at the 2nd European Conference on Analytical Chemistry, 25–30 August, 1975, Budapest, Hungary.     

Characterization of trace elements in medicinal herbs by instrumental neutron activation analysis

Medicinal herbs are often used as alternative medicines for healing and controlling some diseases in the world. This study focuses on the content of heavy and trace elements of some widely consumed herbs in Libya. Nine most popular herbs were analyzed by k ₀-instrumental neutron activation analysis. All the samples, SRM and flux monitors were irradiated for 7 and 10 hours under thermal neutron flux of 1.3·10¹³ cm⁻²·s⁻¹ at Tajoura nuclear reactor. In total, 33 elements were analyzed in different herbs. The variations in the concentration of the elements are attributed to soil composition and the climate in which the plant grows. The study showed that the toxic elements found in the samples were below the levels prescribed by health regulations. The precision and the accuracy of the results were evaluated by analyzing the reference materials Pine Needles SRM 1575 and Citrus Leaves SRM1572.     

BCR certified reference materials for reactor neutron dosimetry

A series of reference materials intended for use as activation or fission monitors for neutron fluence rate measurements has been prepared by the Joint Research Centre of the European Commission. Certification has been carried out by expert European laboratories and distribution of the certified reference materials (CRMs) is through the BCR programme of the Commission. The list (18 CRMs) includes materials to cover the complete energy spectrum, and suitable for different irradiation times. Fission monitors are ²³⁸UO₂ or ²³⁷NpO₂ in the form of microspheres. Activation monitors are high purity metals (Ni, Cu, Al, Fe, Nb, Rh, or Ti), certified for interfering trace impurities, or dilute aluminium-based alloys, where aluminium is chosen as a suitable matrix for reducing the neutron self-shielding effect. Newly certified materials are IRMM-530R Al-0.1%Au, replacing the exhausted IRMM-530 material, used as comparator for k ₀-standardization, and three new Al-Co alloys (0.01-1%Co). Two others, in the process of certification are Al-0.1%Ag and Al-2%Sc for thermal and epithermal fluence rate measurements. Other candidate reference materials currently being certified are two uranium-doped glass intended for dosimetry by the fission-track technique.