Title: Rapid concentration and isotopic measurements of ultra-trace 235U fission products with comparison to an ORIGEN isotope depletion model

Journal Article · · Talanta

We introduce the application of an automated online separation–direct analysis method, RAPID (Rapid Analysis of Post-Irradiation Debris), for the simultaneous measurement of both radioactive and stable fission isotopes from an irradiated highly-enriched uranium target. Developed for the measurement of the concentration and isotopic composition of over 40 elements down to the femtogram level, the RAPID method possesses the sensitivity, stability, and precision needed to achieve accurate, low-level analyses of elements of non-natural origin. The isotopic compositions and concentrations of key fission elements cesium, strontium, yttrium, lanthanum, cerium, praseodymium, neodymium, promethium, and samarium have been measured repeatedly over a six-week period. The validity of these measurements was confirmed using ORIGEN (Oak Ridge Isotope GENeration), an isotope depletion and decay modeling software, to within 1–3%.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
Defense Threat Reduction Agency (DTRA); USDOE; USDOE National Nuclear Security Administration (NNSA)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1542219
Journal Information:
Talanta, Journal Name: Talanta Journal Issue: C Vol. 205; ISSN 0039-9140
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

References (48)

Radionuclide detection by ion-chromatography and on-line ICP/MS and beta detection: Fission product rare earth element measurements journal July 1995
Analysis of high burnup spent nuclear fuel by ICP-MS journal February 2005
Instrumental neutron activation analysis in geochemistry: Emphasis on spectral and uranium fission product interferences journal August 2005
Experimental measurements of short-lived fission products from uranium, neptunium, plutonium and americium journal July 2009
Constraints on fallout melt glass formation from a near-surface nuclear test journal July 2014
Challenges in preparing soil samples and performing a reliable plutonium isotopic analysis by ICP-MS journal August 2014
Determination of short-lived fission product yields with gamma spectrometry journal February 2015
Cumulative fission yields of short-lived isotopes under natural-abundance-boron-carbide-moderated neutron spectrum journal April 2015
Rapid measurements of 235U fission product isotope ratios using an online, high-pressure ion chromatography inductively coupled plasma mass spectrometry protocol with comparison to isotopic depletion models journal February 2019
Quantification of uranium, thorium and gadolinium spectral interferences in instrumental neutron activation analysis of samarium journal April 1987
Validation of the ORIGEN-S code for predicting radionuclide inventories in used CANDU fuel journal May 1995
Ion chromatography with inductively coupled plasma mass spectrometry, a powerful analytical tool for complex matrices journal May 2003
Use of ion chromatography for the determination of fission products and actinides in nuclear applications journal November 1997
A preliminary study for the determination of long-lived radionuclides (second transition group 4-d) in environmental samples by ion chromatography inductively coupled plasma-mass spectrometry (IC-ICP-MS) journal December 2000
Rapid determination of 135Cs and precise 135Cs/137Cs atomic ratio in environmental samples by single-column chromatography coupled to triple-quadrupole inductively coupled plasma-mass spectrometry journal February 2016
Validation of new depletion capabilities and ENDF/B-VII data libraries in SCALE journal August 2012
Re-evaluation of spent nuclear fuel assay data for the Three Mile Island unit 1 reactor and application to code validation journal January 2016
Determination of plutonium isotopes in freshwater lake sediments by sector-field ICP-MS after separation using ion-exchange chromatography journal August 2008
Development of a fast and efficient analytical technique for the isotopic analysis of fission and actinide elements in environmental matrices journal February 2019
Isotope ratio analysis of actinides, fission products, and geolocators by high-efficiency multi-collector thermal ionization mass spectrometry journal September 2009
237 Np analytical method using 239 Np tracers and application to a contaminated nuclear disposal facility journal June 2017
Fission Product Yields from Fission Spectrum n+239Pu for ENDF/B-VII.1 journal December 2010
A generalized method for characterization of 235U and 239Pu content using short-lived fission product gamma spectroscopy
  • Knowles, Justin; Skutnik, Steven; Glasgow, David
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 833 https://doi.org/10.1016/j.nima.2016.06.112
journal October 2016
SRIM – The stopping and range of ions in matter (2010)
  • Ziegler, James F.; Ziegler, M. D.; Biersack, J. P.
  • Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 268, Issue 11-12 https://doi.org/10.1016/j.nimb.2010.02.091
journal June 2010
ASTEC V2 severe accident integral code: Fission product modelling and validation journal June 2014
Actinide targets for the synthesis of super-heavy elements journal December 2015
Mass spectrometry for the determination of fission products 135Cs, 137Cs and 90Sr: A review of methodology and applications journal May 2016
Bk and Cf chromatographic separation and 249Bk/248Cm and 249Cf/248Cm elemental ratios determination by inductively coupled plasma quadrupole mass spectrometry journal March 2013
High precision direct analysis of magnesium isotope ratio by ion chromatography/multicollector-ICPMS using wet and dry plasma conditions journal April 2017
Nuclear Forensics: Scientific Analysis Supporting Law Enforcement and Nuclear Security Investigations journal January 2016
Separation of spectral and non-spectral interferences by on-line high performance ion chromatography inductively coupled plasma sector field mass spectrometry (HPIC-ICP-SFMS) for accurate determination of 234U , 235U, 238U and 232Th in industrial ores journal January 2000
Measurement of strontium isotope ratios by MC-ICP-MS after on-line Rb–Sr ion chromatography separation journal January 2008
Neodymium isotope ratio measurements by LC-MC-ICPMS for nuclear applications: investigation of isotopic fractionation and mass bias correction journal January 2015
Usability of online-coupling ion exchange chromatography ICP-AES/-MS for the determination of trivalent metal complex species under acidic conditions journal January 2016
On-line separation of strontium from a matrix and determination of the 87 Sr/ 86 Sr ratio by Ion Chromatography/Multicollector-ICPMS journal January 2016
Extraction and determination of Cs in natural waters by ICP-MS after ion exchange separation journal January 2004
Rapid fingerprinting of 239Pu and 240Pu in environmental samples with high U levels using on-line ion chromatography coupled with high-sensitivity quadrupole ICP-MS detection journal January 2007
Sm isotope composition and Sm/Eu ratio determination in an irradiated 153Eu sample by ion exchange chromatography-quadrupole inductively coupled plasma mass spectrometry combined with double spike isotope dilution technique journal January 2011
Determination of fission products and actinides in spent nuclear fuels by isotope dilution ion chromatography inductively coupled plasma mass spectrometry journal January 1995
Measurements of extinct fission products in nuclear bomb debris: Determination of the yield of the Trinity nuclear test 70 y later journal July 2016
Application of Ion Chromatography with ICP-MS or MS Detection to the Determination of Selected Halides and Metal/Metalloids Species journal April 2011
Yields of short-lived fission products produced following 235 U ( n th , f ) journal August 1998
Validation of Minor Actinide Cross Sections by Studying Samples Irradiated for 492 Days at the Dounreay Prototype Fast Reactor—I: Radiochemical Analysis journal June 2003
Calculated Activities and Abundances of U 235 Fission Products journal March 1959
Isotopic Depletion and Decay Methods and Analysis Capabilities in SCALE journal May 2011
Isotopic compositions of the elements 1997 (Technical Report) journal January 1998
Measurements of Actinide-Fission Product Yields in Caliban and Prospero Metallic Core Reactor Fission-Neutron Fields journal April 2012
Separation of actinide redox species with cation exchange chromatography and its application to the analysis of spent fuel leaching solutions journal January 2001

Cited By (1)

Rare Earth Element Determination in Uranium Ore Concentrates Using Online and Offline Chromatography Coupled to ICP-MS journal January 2020