RESUMEN

In the frame of the accountancy measurements of the fissile materials, reliable determinations of the plutonium and uranium content in spent nuclear fuel are required to comply with international safeguards agreements. Large-sized dried (LSD) spikes of enriched 235U and 239Pu for isotope dilution mass spectrometry (IDMS) analysis are routinely applied in reprocessing plants for this purpose. A correct characterisation of these elements is a pre-requirement for achieving high accuracy in IDMS analyses. This paper will present the results of external verification measurements of such LSD spikes performed by the European Commission and the International Atomic Energy Agency.

RESUMEN

The IRMM-1000a and IRMM-1000b uranium reference materials, of 20 and 50 mg uranium, respectively, were produced by the European Commission Joint Research Centre's Institute for Reference Materials and Measurements (EC-JRC-IRMM) in collaboration with the Institute for Transuranium Elements (EC-JRC-ITU). They are novel uranium reference materials certified for the production date based on the 230Th/234U radiochronometer, i.e. the date of the last chemical separation of these two radionuclides. The certified reference value and its uncertainty, homogeneity and stability of the material were established in accordance with the ISO Guide 34:2009 and the 'Guide to the Expression of Uncertainty in Measurement'.

RESUMEN

The Institute for Reference Materials and Measurements (IRMM) has extensive experience in the development of isotopic reference materials and the organization of interlaboratory comparisons (ILC) for nuclear measurements in compliance with the respective international guidelines (ISO Guide 34:2009 and ISO/IEC 17043:2010). The IRMM Nuclear Signatures Interlaboratory Measurement Evaluation Program (NUSIMEP) is an external quality control program with the objective of providing materials for measurements of trace amounts of nuclear materials in environmental matrices. Measurements of the isotopic ratios of the elements uranium and plutonium in small amounts, typical of those found in environmental samples, are required for nuclear safeguards and security, for the control of environmental contamination and for the detection of nuclear proliferation. The measurement results of participants in NUSIMEP are evaluated according to international guidelines in comparison to independent external certified reference values with demonstrated metrological traceability and uncertainty. NUSIMEP-7 focused on measurements of uranium isotope amount ratios in uranium particles aiming to support European Safeguards Directorate General for Energy (DG ENER), the International Atomic Energy Agency's (IAEA) network of analytical laboratories for environmental sampling (NWAL) and laboratories in the field of particle analysis. Each participant was provided two certified test samples: one with single and one with double isotopic enrichment. These NUSIMEP test samples were prepared by controlled hydrolysis of certified uranium hexafluoride in a specially designed aerosol deposition chamber at IRMM. Laboratories participating in NUSIMEP-7 received the test samples of uranium particles on two graphite disks with undisclosed isotopic ratio values n((234)U)/n((238)U), n((235)U)/n((238)U) and n((236)U)/n((238)U). The uranium isotope ratios had to be measured using their routine analytical procedures. Measurement of the major ratio n((235)U)/n((238)U) was obligatory; measurement of the minor ratios n((234)U)/n((238)U) and n((236)U)/n((238)U) was optional. Of the twenty-four institutes that registered for NUSIMEP-7, 17 have reported their results achieved by different analytical methods. The results of NUSIMEP-7 confirm the capability of laboratories in measuring n((234)U)/n((238)U), n((235)U)/n((238)U) and n((236)U)/n((238)U) in uranium particles of the size below 1 µm diameter. Furthermore, they underpin the recent advances in instrumental techniques in the field of particle analysis. In addition, feedback from the measurement communities from nuclear safeguards, nuclear security and earth sciences was collected in view of identifying future needs for NUSIMEP interlaboratory comparisons.

Asunto(s)

Uranio/análisis , Laboratorios , Tamaño de la Partícula , Control de Calidad , Monitoreo de Radiación/normas , Estándares de Referencia , Reproducibilidad de los Resultados , Incertidumbre , Uranio/química , Uranio/normas

RESUMEN

Confidence in comparability and reliability of measurement results in nuclear material and environmental sample analysis are established via certified reference materials (CRMs), reference measurements, and inter-laboratory comparisons (ILCs). Increased needs for quality control tools in proliferation resistance, environmental sample analysis, development of measurement capabilities over the years and progress in modern analytical techniques are the main reasons for the development of new reference materials and reference methods for nuclear safeguards and security. The Institute for Reference Materials and Measurements (IRMM) prepares and certifices large quantities of the so-called "large-sized dried" (LSD) spikes for accurate measurement of the uranium and plutonium content in dissolved nuclear fuel solutions by isotope dilution mass spectrometry (IDMS) and also develops particle reference materials applied for the detection of nuclear signatures in environmental samples. IRMM is currently replacing some of its exhausted stocks of CRMs with new ones whose specifications are up-to-date and tailored for the demands of modern analytical techniques. Some of the existing materials will be re-measured to improve the uncertainties associated with their certified values, and to enable laboratories to reduce their combined measurement uncertainty. Safeguards involve the quantitative verification by independent measurements so that no nuclear material is diverted from its intended peaceful use. Safeguards authorities pay particular attention to plutonium and the uranium isotope (235)U, indicating the so-called 'enrichment', in nuclear material and in environmental samples. In addition to the verification of the major ratios, n((235)U)/n((238)U) and n((240)Pu)/n((239)Pu), the minor ratios of the less abundant uranium and plutonium isotopes contain valuable information about the origin and the 'history' of material used for commercial or possibly clandestine purposes, and have therefore reached high level of attention for safeguards authorities. Furthermore, IRMM initiated and coordinated the development of a Modified Total Evaporation (MTE) technique for accurate abundance ratio measurements of the "minor" isotope-amount ratios of uranium and plutonium in nuclear material and, in combination with a multi-dynamic measurement technique and filament carburization, in environmental samples. Currently IRMM is engaged in a study on the development of plutonium reference materials for "age dating", i.e. determination of the time elapsed since the last separation of plutonium from its daughter nuclides. The decay of a radioactive parent isotope and the build-up of a corresponding amount of daughter nuclide serve as chronometer to calculate the age of a nuclear material. There are no such certified reference materials available yet.

Asunto(s)

Plutonio/normas , Monitoreo de Radiación/normas , Uranio/normas , Espectrometría de Masas/métodos , Plutonio/análisis , Control de Calidad , Estándares de Referencia , Reproducibilidad de los Resultados , Uranio/análisis

RESUMEN

Uranium and plutonium particulate test materials are becoming increasingly important as the reliability of measurement results has to be demonstrated to regulatory bodies responsible for maintaining effective nuclear safeguards. In order to address this issue, the Institute for Reference Materials and Measurements (IRMM) in collaboration with the Institute for Transuranium Elements (ITU) has initiated a study to investigate the feasibility of preparing and characterizing a uranium particle reference material for nuclear safeguards, which is finally certified for isotopic abundances and for the uranium mass per particle. Such control particles are specifically required to evaluate responses of instruments based on mass spectrometric detection (e.g. SIMS, TIMS, LA-ICPMS) and to help ensuring the reliability and comparability of measurement results worldwide. In this paper, a methodology is described which allows quantifying the uranium mass in single micron particles by isotope dilution thermal ionization mass spectrometry (ID-TIMS). This methodology is characterized by substantial improvements recently achieved at IRMM in terms of sensitivity and measurement accuracy in the field of uranium particle analysis by TIMS. The use of monodisperse uranium oxide particles prepared using an aerosol generation technique developed at ITU, which is capable of producing particles of well-characterized size and isotopic composition was exploited. The evidence of a straightforward correlation between the particle volume and the mass of uranium was demonstrated in this study. Experimental results have shown that the uranium mass per particle can be measured via the ID-TIMS method to a relative expanded uncertainty of about 10% (coverage factor k=2). The availability of reliable and validated methods for the characterization of uranium particles is considered to be essential for the establishment of SI-traceable measurement results. It is therefore expected that the method developed in this study is valuable for the certification of particulate materials in which the isotopic composition and the content of uranium must be accurately known.

RESUMEN

A method is described that allows measuring the isotopic composition of small uranium oxide particles (less than 1µm in diameter) for nuclear safeguards purposes. In support to the development of reliable tools for the identification of uranium and plutonium signatures in trace amounts of nuclear materials, improvements in scanning electron microscopy (SEM) and thermal ionization mass spectrometry (TIMS) in combination with filament carburization and multiple ion counting (MIC) detection were investigated. The method that has been set up enables the analysis of single particles by a combination of analytical tools, thus yielding morphological, elemental and isotopic information. Hereby individual particles of certified reference materials (CRMs) containing uranium at femtogram levels were analysed. The results showed that the combination of techniques proposed in this work is suitable for the accurate determination of uranium isotope ratios in single particles with improved capabilities for the minor abundant isotopes.