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Laboratory for nuclear forensics and environmental analysis

Laboratory for nuclear forensics and environmental analysis . Presented by: Éva Széles Seminar on R & D Activities at the Institute of Isotopes Related to Nuclear Security February 19, 2010 , Vienna. www.iki.kfki.hu. Main Tasks of the Laboratory.

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Laboratory for nuclear forensics and environmental analysis

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  1. Laboratory for nuclear forensics and environmental analysis Presented by: Éva Széles Seminar on R & D Activities at the Institute of Isotopes Related to Nuclear Security February 19, 2010, Vienna www.iki.kfki.hu

  2. Main Tasks of the Laboratory Analysis of confiscated nuclear materials – nuclear forensics characterization and identification of the found and confiscated samples with unknown origin destructive and non-destructive analysis analysis of U and Pu  e.g. precise isotope ratio measurements Analysis for safeguards purposes environmental and swipe samples single particle analysis by laser ablation ICP-MS (LA-ICP-MS) environmental monitoring for safeguards purposes before the decomissioning of nuclear facilities

  3. Main Tasks of the Laboratory • Analysis of environmental samples - other aspects • Measurement of low-level actinides in environmental samples (soil, sediment, water, plant, etc.) • Analysis of alternative nuclear materials (Am, Np, Cm) • Direct analysis of solid samples by LA-ICP-MS technique (e.g. geological samples, uranium ore samples, metal samples, etc.)

  4. Applied Techniques Main instruments: • High resolution inductively coupled plasma sector-field mass spectrometry (ICP-SFMS) • High resolution gamma spectrometry (HRGS) • Scanning electron microscope (SEM/EDX) • Neutron coincidence counting (NCC) Additional techniques: • X-ray diffraction analysis (XRD) • Prompt-gamma activation analysis (PGAA)

  5. High-resolution inductively coupled plasma sector-field mass spectrometer (ICP-SFMS) • ELEMENT2 with single collector • Installed in a clean room (Class 100 000) • Various sample introduction systems: • Stable sample introduction • Laser ablation system • Sample preparation laboratory (Class 10 000): • With a Class 100 laminar flow hood Ultra-trace level measurements

  6. Laser ablation (LA) unit for the mass spectrometer • Quasi non-destructive measurement • no chemical sample preparation needed • short analysis time(typically <1 h/sample) Laser ablation system: UP213 (New Wave)

  7. High-resolution gamma spectrometry (HRGS) • Fully non-destructive measurement • No sample preparation needed • Low-background gamma spectrometer • Iron chamber with 20 cm wall thickness • 150 cm3 coaxial HPGe detector • 34% relative efficiency • Sample cavity flushed with nitrogen • Planned upgrades: • Better detector • Underground facility • Low-energy planar HPGe detectors • For U and Pu isotopics N2 flushing

  8. Scanning Electron Microscope (SEM) • Type JEOL JSM-5600LV • Broad magnification rangeup to 300 000 • “Low vacuum” mode for observing nonconductive samples in their nativestate • Elemental analysis • Attached energy dispersive X-ray spectrometer (EDS)

  9. Origin of nuclear forensics in Hungary Illicit trafficking in Hungary: since the early ’90s • In the beginning: only planar HPGe used • Since then: • Low-background HPGe • SEM • ICP-MS • NCC A possible site of illicit trafficking in Budapest

  10. Nuclear forensic applications at IKI • Tested with following nuclear materials: • Powder (U compounds) • DA & NDA • Pellets (U oxide) • DA & NDA • Fuel rods (U oxide) • NDA • Fuel assemblies • NDA • Sealed sources (eg. Pu) • NDA • … • Non-destructive techniques (NDA) are still needed though very accurate destructive methods (DA) are available

  11. Selected nuclear forensic applications developed at the Institute of Isotopes

  12. Determination of production date of nuclear materials Uranium age dating bydestructive ICP-MS • Digestion of the uranium-oxide sample • Determination of234U-content by isotope dilution ICP-MS analysis • Determination of230Th-content by isotope dilution ICP-MS analysis after extraction-chromatographic separation • Production of229Th tracer: from 233U-solution („milking”) Uranium age dating byquasi-non destructiveLA-ICP-MS

  13. Uranium age dating byfully non-destructive HRGS • Two measurements: • 234U/238U by planar HPGe • 214Bi/238U by coaxial HPGein low background • Activity ratios determined by relative (“intrinsic”) efficiency calibration • Independent of measurement geometry

  14. Detecting the presence of reprocessed uranium  232U analysis by HRGS • 232U content indicates reprocessed uranium 232U content determined by HRGS as a function of 235U enrichment 236U and Pu isotopes can be measured by ICP-MS

  15. Rare-earth elements in uranium-bearing materials determined by ICP-SFMS – Origin assessment Three uranium ore concentrates originating from different mills in order to compare their REE profiles after digestion of the samples and separation of the matrix (U)

  16. Trace elements in uranium-oxide determined by ICP-SFMS – Origin assessment Trace element analysis in 3 confiscated uranium-oxid pellets  Joint analysis with Institute for Transuranium Elements (ITU) • Samples: • 590: Natural (HU-NAT) • 642: LEU (HU-LEU) • 643: DU (HU-DEP) sample 590

  17. Quality assurance • ISO 9001:2000 • ISO/IEC 17025 – accreditation of the ICP-MS laboratory is in progress • Participation in interlaboratory comparisons and proficiency tests • ITWG - HEU • REIMEP, NUSIMEP, IAEA-PT • Joint analysis with JRC ITU, Karlsruhe

  18. Inter-laboratory comparison (Round Robin) organised by the ITWG (2001) • More than 10 nuclear forensic laboratories participated • ~1 g HEU sample/lab. Isotopic composition Production date

  19. Joint analysis with Institute for Transuranium Elements (ITU) • 3 uranium oxide pellets from 3 different batches were analysed at IKI by HRGS and LA-ICP-SFMS • The pellets were sent to ITU for further investigation using DA methods ITU IKI

  20. Safeguards analysis of environmental samples

  21. Analysis of swipe samples– bulk analysis The laboratory is capable of determining ultra-trace amounts of uranium and plutonium isotopes and their precise isotope ratios in environmental swipe samples Analytical procedures developed for bulk analysis: Screening by gamma spectrometry Microwave digestion instead of ashing Extraction chromatographic separation with TRU®column process ICP-SFMS measurement Detection limits achieved: Uranium: 0.01 – 5 ng (IAEA SAL req.: 0.1 - 5 ng) Plutonium: 1 – 7 fg (IAEA SAL req.: 10 fg) Special developments: reduction of procedure background Clean room facilities Optimized procedure Sub-boiled acids and minimal chemical consumption Method was tested by analysis of real swipe samples

  22. Analytical performanceparameters achieved

  23. Analysis of single particles by LA-ICP-MS technique Development of a novel methodology for the isotopic composition measurement of single particles • Current results:Isotopic analysis of individual uranium particles by laser ablation ICP-SFMS • Tested for uranium-oxide particles with different enrichment, lateral dimensions: down to 10 micron • Applicable also for low-abundant isotopes (234U, 236U) • Typical precision achieved: 0.2-5% RSD for 235U/238U • Testing for sub-micron particles (JRC IRMM, NUSIMEP) • Particle location: fission track and SEM/EDS  Further aim: adaptation of the method for swipe samples

  24. Analysis of single particles by LA-ICP-MS technique LA-ICP-MS measurement LEU particle (40 x 38 um) SEM/EDS

  25. Provision for decommissioning of nuclear facilities - environmental monitoring Objectives: • determination of the environmentalcontamination baseline/level asa reference database in thevicinity of Hungarian nuclearfacilities • comprehensive environmental monitoring and analysis before decommissioning for safeguards purposes • Test measurements at the KFKI site near the research reactor: • plutonium and uranium concentrations and isotopic ratios in soil and wood-moss were determined • Results: Pu: ~fg/g, U: ~ng/g

  26. Conclusion • IKI is capable of a complete nuclear-forensic characterization of most types of nuclear material • Combined use of DA and NDA instrumentation • HRGS, ICP-SFMS, SEM, NCC • Note on Pu: handling only sealed sources • Only NDA can be applied • Environmental measurements at ultra-trace level

  27. Conclusion • Planned developments: • Particle analysis with laser ablation ICP-MS • Upgrading the low-background HRGS facilities • Possible future application: In-field age dating of shielded HEU (e.g. of an Improvised Nuclear Device)?

  28. www.iki.kfki.hu Thank You for Your attention! Section Head: Dr. András Kovács Staff: Staff on-leave: ICP-MS:ICP-MS: Dr. Tamás Bíró Dr. Zsolt Stefánka (HAEA) Dr. Éva Széles Dr. Zsolt Varga (ITU) Mr. Róbert Katona Ms. Zsuzsanna Mácsik HRGS: HRGS: Dr. László Lakosi Dr. József Zsigrai (ITU) Dr. Nguyen Cong Tam Mr. János Bagi (JRC Ispra) Mr. István Almási Mr. Péter Nagy SEM: Dr. Péter Hargittai

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