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

Abstract

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:
Research Org.:
Idaho National Lab. (INL), Idaho Falls, ID (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
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
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

Citation Formats

Snow, Mathew S., Snyder, Darin C., Mann, Nick R., and White, Byron M. Method for ultra-trace cesium isotope ratio measurements from environmental samples using thermal ionization mass spectrometry. United States: N. p., 2015. Web. doi:10.1016/j.ijms.2015.03.006.
Snow, Mathew S., Snyder, Darin C., Mann, Nick R., & White, Byron M. Method for ultra-trace cesium isotope ratio measurements from environmental samples using thermal ionization mass spectrometry. United States. doi:10.1016/j.ijms.2015.03.006.
Snow, Mathew S., Snyder, Darin C., Mann, Nick R., and White, Byron M. Fri . "Method for ultra-trace cesium isotope ratio measurements from environmental samples using thermal ionization mass spectrometry". United States. doi:10.1016/j.ijms.2015.03.006.
@article{osti_1182691,
title = {Method for ultra-trace cesium isotope ratio measurements from environmental samples using thermal ionization mass spectrometry},
author = {Snow, Mathew S. and Snyder, Darin C. and Mann, Nick R. and White, Byron M.},
abstractNote = {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.},
doi = {10.1016/j.ijms.2015.03.006},
journal = {International Journal of Mass Spectrometry},
number = C,
volume = 381-382,
place = {United States},
year = {Fri May 01 00:00:00 EDT 2015},
month = {Fri May 01 00:00:00 EDT 2015}
}