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Title: Method for ultra-trace cesium isotope ratio measurements from environmental samples using thermal ionization mass spectrometry

135Cs/137Cs isotope ratios can provide the age, origin and history of environmental Cs contamination. Relatively high precision 135Cs/137Cs isotope ratio measurements from samples containing femtogram quantities of 137Cs are needed to accurately track contamination resuspension and redistribution following environmental 137Cs releases; however, mass spectrometric analyses of environmental samples are limited by the large quantities of ionization inhibitors and isobaric interferences which are present at relatively high concentrations in the environment. We report a new approach for Cs purification from environmental samples. An initial ammonium molybdophosphate-polyacrylonitrile (AMP-PAN) column provides a robust method for extracting Cs under a wide variety of sample matrices and mass loads. Cation exchange separations using a second AMP-PAN column result in more than two orders of magnitude greater Cs/Rb separation factors than commercially available strong cation exchangers. Coupling an AMP-PAN cation exchanging step to a microcation column (AG50W resin) enables consistent 2-4% (2σ) measurement errors for samples containing 3-6,000 fg 137Cs, representing the highest precision 135Cs/137Cs ratio measurements currently reported for soil samples at the femtogram level.
Authors:
 [1] ;  [2] ;  [2] ;  [2]
  1. Washington State Univ., Pullman, WA (United States). Dept. of Chemistry; Idaho National Lab. (INL), Idaho Falls, ID (United States)
  2. Idaho National Lab. (INL), Idaho Falls, ID (United States)
Publication Date:
OSTI Identifier:
1182691
Report Number(s):
INL/JOU--14-31760
Journal ID: ISSN 1387-3806; TRN: US1500195
DOE Contract Number:
AC07-05ID14517; 2012-DN-130-NF0001-02
Resource Type:
Journal Article
Resource Relation:
Journal Name: International Journal of Mass Spectrometry; Journal Volume: 381-382; Journal Issue: C
Publisher:
Elsevier
Research Org:
Idaho National Laboratory (INL), Idaho Falls, ID (United States)
Sponsoring Org:
USDOE National Nuclear Security Administration (NNSA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CESIUM 137; CESIUM 135; MASS SPECTROSCOPY; AMMONIUM COMPOUNDS; MOLYBDOPHOSPHATES; RESINS; ISOTOPE RATIO; NITRILES; ORGANIC POLYMERS; CONCENTRATION RATIO; ION EXCHANGE; ACCURACY; CONTAMINATION; PARTICLE RESUSPENSION; ABUNDANCE; ENVIRONMENT; INTERFERENCE; ORIGIN; PURIFICATION; SOILS; SEPARATION PROCESSES AMP-PAN; TIMS